Synthesis of anthracite networks and environmental superconductors

Abstract

Several variants of synthetic carbon materials are disclosed. The materials can exhibit a variety of properties, including high electrical conductivity. The materials can also have advantageous structural and mechanical properties. They can form a gas-impermeable barrier layer, form insulating structures, and can have unique optical properties.

Description

[0001] Cross-reference to related applications:

[0002] This application claims priority to U.S. Provisional Application No. 63 / 039,525, filed June 16, 2020, the entire disclosure of which is incorporated herein by reference. The following applications are hereby incorporated, in their entirety, by reference for all purposes: U.S. Provisional Patent Application 63 / 039,525 ('525 application); U.S. Provisional Patent Application 63 / 129,154 ('154 application); U.S. Provisional Patent Application 63 / 075,918 ('918 application); U.S. Provisional Patent Application 63 / 806,760 ('760 application); U.S. Provisional Patent Application 63 / 121,308 ('308 application); U.S. Utility Model Application 16 / 758,580 ('580 application); U.S. Utility Model Application 16 / 493,473 ('473 application); PCT / US17 / 17537 ('17537 application); and U.S. Patent 10,717,843B2 ('843B2 patent). Technical Field

[0003] This disclosure relates to novel methods for constructing microscopic or macroscopic objects from anthracite networks exhibiting molecular-scale two-dimensionality. In particular, this disclosure relates to novel methods for constructing anthracite networks from different types of two-dimensional building blocks (including carbonaceous and non-carbonaceous types).

[0004] This disclosure also relates to novel synthetic anthracite networks crosslinked via structural dislocations. In particular, this disclosure relates to coating materials and frameworks comprising a hierarchically crosslinked synthetic anthracite network obtained via structural dislocations.

[0005] Finally, this disclosure also relates to novel methods for inducing a superconducting state in a material under environmental conditions, and novel environmental superconductors. Background Technology

[0006] Two-dimensional structures at the molecular scale (such as graphene-carbon) have demonstrated excellent properties. However, to facilitate the practical use of these two-dimensional structures in many macroscopic or even microscopic applications, they must be used to construct hierarchical materials that are three-dimensional at a larger scale. Constructing these hierarchical materials that are two-dimensional at the molecular scale and three-dimensional at a higher scale has proven challenging.

[0007] A common approach to constructing larger-scale systems is to bring two-dimensional lattices—typically graphene lattices—into contact with each other and cohede them into systems comprising multiple lattices. Such systems (comprising multiple distinct two-dimensional lattice members) are described in this disclosure as “assemblies.” Macroscopic three-dimensional assemblies can be readily constructed from two-dimensional lattices.

[0008] In assemblages, two-dimensional lattice members typically cohede with each other at regions where they make overlapping van der Waals (“vdW”) contacts. Such systems are primarily cohesive through intermolecular forces at these contacts. We describe this type of assembly (where the primary cohesive mechanism is the intermolecular force between members at vdW contacts) as a “vdW assembly.” VdW assemblages, regardless of their physical architecture, share the common property of system-level covalent discontinuity.

[0009] Intermolecular forces are weaker than covalent bonds, and the weak cohesion allows overlapping members of vdW assemblies to slide over each other. This tendency for shear yielding limits the modulus of graphitic carbon and softens it. Since the intermolecular forces between two lattice elements vary with their contact area and contact distance, vdW assemblies with small lattice members are typically particularly weak.

[0010] In other assemblies, multiple two-dimensional lattice members can be cohesively linked primarily by chemical bonding forces. In such bonded assemblies, the chemical bonding forces between individual lattice members suppress shear yielding and make the assemblies more robust than vdW assemblies, which are cohesive solely by intermolecular forces. In the prior art, bonded assemblies are formed by chemically altering the surface of the graphene lattice, for example, through graft chains to the graphene lattice, which can then be used to crosslink the graphene lattice to other lattices. While this represents an improvement over vdW assemblies, the bonding between bonded lattice members still limits the realization of universal two-dimensional molecular structures.

[0011] In principle, some limitations of assemblies can be overcome by constructing “graphene networks,” which, as described in this paper, are structures with two-dimensional molecular-scale geometry that are three-dimensionally cross-linked at some scale. Based on the cross-linking and network geometry of graphene networks, they cannot be destroyed without disrupting a portion of their two-dimensional molecular structure. Intuitively, this should be the best way to construct common objects, typically with macroscopic dimensions, that exhibit properties similar to two-dimensional structures. These objects would benefit if the network geometry could be reasonably structured.

[0012] One source of inspiration for constructing graphene networks is anthracite, a naturally occurring mature coal, which includes “anthracite networks.” Anthracite networks are described in this paper as hierarchical graphene networks with three-dimensional cross-linking via certain characteristic dislocations (“anthracite dislocations”) and where z-adjacent layers are arranged in a nematic pattern. These three-dimensionally cross-linked anthracite networks are generated when organic matter is exposed to high temperatures and pressures during geological periods. As the organic matter matures, its carbon content increases, and its molecular structure becomes increasingly dominated by a two-dimensional polycyclic layout of carbon, which eventually coalesces upon evolving structural dislocations. These structural dislocations provide the multicyclic cross-linking between these multicyclic layouts (thus creating a monolithic multicyclic network).

[0013] Several types of anthracite dislocations exist for crosslinking anthracite networks. One type is described herein as a “Y dislocation.” In short, a Y dislocation is formed when an atomic monolayer branches into an atomic bilayer, where the intersections include multi-ringed loops (things we describe as multi-ringed loops may include multiple orbital hybridization states, although the term “multi-ringed” is generally applied to pure sp[s]. 2 (Hybridized polycyclic structure). The second type of anthracite dislocation is the screw dislocation, which consists of a multi-layered helical arrangement of atomic monolayers. Other anthracite dislocations may contain elements of both Y dislocations and screw dislocations. All these dislocations contribute to the formation of transverse and vertical polycyclic molecular-scale crosslinks between the two-dimensional molecular structures. This three-dimensional molecular-scale crosslinking has a hardening and stiffening effect on the anthracite network, which is why anthracite is sometimes called "hard coal."

[0014] While the crosslinking of natural anthracite makes it an interesting example of macroscopic graphene networks, it has practical limitations. Due to the geological composition of anthracite, organic and inorganic inclusions can be embedded as secondary phases. No engineering control is performed during the formation process, making it impossible to avoid defects and apply rational design principles. These drawbacks significantly limit the usefulness of anthracite in fuel applications, but it is possible to overcome these limitations if synthetic anthracite networks could be fabricated. Exemplary synthetic methods are detailed in applications '760 and '918, in which coated frameworks are synthesized using template-guided chemical vapor deposition (“CVD”) or methods described in those applications as “surface replication”. If rationally designed coated frameworks crosslinked through anthracite dislocations can be constructed, these synthesized geologically mimicry frameworks would represent an improvement over natural anthracite.

[0015] In existing technologies, non-anthracite graphene networks constructed from two-dimensional materials have been demonstrably demonstrated through surface replication. Small Schwarzite-like graphene networks appear to have been synthesized using CVD deposition on zeolite Y template particles. Zeolite Y is considered to have a supercage diameter of approximately... The larger pore size of zeolite Y provides improved internal gas diffusion compared to smaller pore zeolites, but the micropores of zeolite Y still appear to be small enough that the space confinement effect causes the grown graphene lattice to aggregate into a single continuous graphene network, which is three-dimensionally cross-linked but not generated by anthracite dislocations.

[0016] The spatial confinement within the pores of microporous zeolites appears to force lattice aggregation, but it also presents significant challenges. One problem is that deposited carbon tends to clog the pores of the zeolite template, prematurely terminating deposition within the template. Consequently, carbon templated with zeolite is rarely intact. Another issue is the extremely slow and diffusion-restricted deposition kinetics throughout the microporous template. The maximum template depth for which a substantially intact Schwarz structure network has been demonstrated (as evidenced by an average of 72 carbon atoms per zeolite supercage) is only about 20 nm. Even at such a shallow depth, deposition on zeolite Y nanoparticles requires 6 hours to complete.

[0017] Beyond these challenges, Schwarz structures may suffer from another fundamental drawback: they approximate Schwarz minimal surface geometries. While theoretical work supports the goal of generating graphene networks modeled on these surfaces, we demonstrate here that minimal surface geometries may not be as suitable as the denser hierarchical architectures of anthracite networks due to the minimal nature of these surfaces. Specifically, we find that the geometry of Schwarz structures can constrain or effectively eliminate interlayer vdW interactions that contribute to system cohesion in hierarchical anthracite networks. For this reason, rather than sacrificing vdW cohesion for molecular-scale density reduction, we prefer to achieve density reduction through hierarchical, larger-scale pore engineering, as demonstrated by the tunable mesopore or macropore-encapsulated frameworks described in applications '760 and '918.

[0018] In addition to Schwarz-like network structures, we speculate that the prior art may include instances of synthetic graphene networks that have not yet been recognized. This speculation is based on the analyses and concepts developed and refined in this disclosure, and the analyses are discussed in more detail below.

[0019] In one instance, based on our own post-hoc analysis, we found evidence that a graphene network can be constructed on a MgO template by grafting the edges of graphite domains grown on the surface of a MgO template together [1]. Prior to extracting the content MgO, the coated carbon phase formed on the MgO consists of an atomic monolayer. Since anthracite dislocations consist of interlayer crosslinks of multiple z-adjacent layers, they cannot exist in a monolayer, and our post-hoc analysis found that this network lacks anthracite dislocations as it is characterized as a monolayer coated phase on the template surface. Therefore, its molecular-scale crosslinks are only lateral or intralayer, and this anisotropy prevents the framework from realizing some of the fundamental benefits associated with more three-dimensional molecular-scale crosslinks (e.g., stiffness and structural rigidity). Thus, upon extracting the content template and drying the coated framework, the pores within the framework collapse, resulting in a dried post-graphene network with bilayer structuring but without the interlayer molecular-scale crosslinks of these bilayers that anthracite dislocations can provide.

[0020] In another instance, we found evidence that nano-onions grown with metal catalysts comprise graphene networks in which substantially parallel z-adjacent graphene layers (i.e., a more ordered arrangement than the nematic arrangement found in anthracite networks) are vertically cross-linked through anthracite dislocations, but typically with lateral spacing measured to be no less than 5 nm. These large spacings at the nanocrystalline graphite scale make the molecular-scale cross-linking of these graphene networks so anisotropic and lateral that they resemble graphite more than anthracite. Therefore, we describe these graphite-like networks as “graphite networks” and distinguish them from anthracite networks. Like the graphene networks we hypothesize exist in the first instance of the prior art described above, these graphite networks exhibit anisotropic lateral molecular-scale cross-linking. Summary of the Invention

[0021] This disclosure demonstrates methods for synthesizing microscopic or macroscopic anthracite networks by constructing block grafts of two-dimensional molecules together. In particular, these methods can be used to synthesize “x-carbon” and “z-carbon” (two types of anthracite networks whose properties are described in more detail in the text of this application) and other novel graphene networks. These methods may optionally include: synthesizing anthracite networks having non-carbonaceous chemical compositions or comprising compounds. These methods may also optionally include: synthesizing anthracite networks with templated structural features, hierarchical morphology, controllable crosslinking density, and porosity.

[0022] This disclosure also discloses materials including synthetic anthracite networks. These materials include x-carbon and z-carbon. These materials also include synthetic anthracite networks in two-dimensional forms comprising light elements and in two-dimensional forms comprising compounds comprising light elements. Specifically, these materials include BN and BC. x N. These materials include anthracite networks of any morphology, particularly templated morphology. This disclosure also relates to derivatives of these novel materials, such as chemically or physically modified derivatives.

[0023] This disclosure also illustrates methods for inducing a superconducting state in materials and objects under ambient conditions. In particular, these methods may include techniques for shielding materials and objects comprising two-dimensional molecular structures from collisions with gas molecules, including forming an impermeable barrier phase around the material and object while maintaining a vacuum. Optionally, these methods may include placing the material and object in a vacuum.

[0024] This disclosure also illustrates environmentally relevant materials or objects, including environmental superconductors, described in more detail in the text of this application. These environmental superconductors may include materials or objects having a two-dimensional molecular structure. These environmental superconductors may be nanoscale, microscale, or macroscale. Optionally, they may include synthetic anthracite networks. Generally, they may include materials or objects with evacuated liquid or gaseous molecules. In particular, they may include materials or objects having a barrier phase and an internal phase, wherein the internal phase comprises a porous material shielded by the barrier phase from atomic or molecular collisions that would otherwise be encountered in a non-vacuum environment.

[0025] This disclosure also illustrates methods for synthesizing environmentally relevant materials or objects, including environmental superconductors. These methods may include: synthesizing materials or objects comprising two-dimensional molecular structures. In particular, the materials or objects may include anthracite networks. The synthesis of these anthracite networks may include: linking smaller structures into anthracite networks by grafting smaller structures onto each other. These smaller structures may optionally include carbon black or anthracite networks. Attached Figure Description

[0026] Figure 1 This is a classification chart illustrating how graphene networks are categorized in this disclosure. Synthetic anthracite networks, including those containing x-carbon and z-carbon, are highlighted. Each of these categories is further subdivided into sp... x Networks, intermediate networks, or spiral networks, the latter two being connected via sp x It was formed through the maturation of the internet.

[0027] Figure 2 shows a model of a Schwarz structure network, an example of a non-hierarchical graphene network with a helical geometry. A Schwarz surface is shown alongside the model.

[0028] Figure 3 A curved two-dimensional surface is shown, and the tangent xy plane and orthogonal z-axis are identified. The space above and below the curved surface constitutes the z-space.

[0029] Figure 4 This is a molecular model of a bent-ring disordered graphene structure. The structure is rotated as indicated by the arrows to provide multiple perspective views. Enlarged insets show regions of positive and negative Gaussian curvature. Edges in the foreground are highlighted in blue and shown in enlarged insets of their wavy geometry.

[0030] Figure 5 This diagram illustrates two possible scenarios that may occur during the geological encounter between two cyclic ordered graphene structures. Figure 5 In section A, the encounter of geological structures is shown. Figure 5 In section B, the subduction event that produces edge dislocations is shown. The subducted lattice is marked with 'x'. Figure 5In C, the sp-shaped structure that generates edge aggregation to form a new graphene structure is shown. 2 Grafting events produce some slight ring disorder and curvature.

[0031] Figure 6 Five model systems are shown to illustrate the definitions and concepts associated with graphene structures and systems.

[0032] Figure 7 A system of models is shown to illustrate the definitions and concepts associated with the structure of graphene. The models include Y dislocations and highlight the diamond-like joints that form its core.

[0033] Figure 8 Photographs of various equipment used in the program shown in this disclosure are displayed.

[0034] Figure 9 This is a SEM micrograph of the encapsulated framework of sample A1. The translucent areas of the encapsulation wall are circled in yellow.

[0035] Figure 10 Includes TEM micrographs of sample A1 at different magnification levels. At the highest magnification level, the nematic arrangement of the coating walls is shown. The nematic layers are outlined in yellow. Magnified insets show Y dislocations.

[0036] Figure 11 This is another enclosed frame TEM micrograph that further demonstrates the concept of nematic arrangement.

[0037] Figure 12 The illustration is from anthracite literature, showing (A) edge dislocations, (B) Y dislocations, (C) screw dislocations, and (D) screw loops (a pair of screw dislocations).

[0038] Figure 13 This is a portion of the single-point Raman spectrum of sample A1, with regions of interest indicated by yellow circles, such as the unfitted G band (G). u ), unfitted Tr band (Tr) u ), unfitted D-band (D u ) and 1100-1200cm -1 The unfitted shoulder is shown in the inset. The full Raman spectrum of sample A1 is shown in the figure. The spectrum was acquired using a 532 nm laser with a power setting of 2 mW.

[0039] Figure 14 The diagram shows the two fitted peaks (f-1, f-2) of the Raman curve for sample A1, the fitted curve, the actual curve, and the residuals representing the difference between the fitted and actual curves. The peak type, position, height, fwhm, and area of ​​the fitted peaks are also presented in tabular form.

[0040] Figure 15The three fitted peaks (f-1, f-2, f-3) of the Raman curve for sample A1, the fitted curve, the actual curve, and the residuals representing the difference between the fitted and actual curves are shown. The peak type, position, height, fwhm, and area of ​​the fitted peaks are also presented in tabular form.

[0041] Figure 16 The diagram shows the four fitted peaks (f-1, f-2, f-3, f-4) of the Raman curve for sample A1, the fitted curve, the actual curve, and the residuals representing the difference between the fitted and actual curves. The peak type, position, height, peak fwhm, and area of ​​the fitted peaks are also presented in tabular form.

[0042] Figure 17 The diagram shows the two fitted peaks (f-1, f-2, f-3, f-4) of the Raman curve of sample A1 after annealing, the fitted curve, the actual curve, and the residuals representing the difference between the fitted and actual curves. The peak type, position, height, peak fwhm, and area of ​​the fitted peaks are also shown in tabular form.

[0043] Figure 18 It is the XRD line shape of sample A1, where the three fitted peaks are labeled as I, II and III.

[0044] Figure 19 The graphs show the thermal oxidation curves of samples A1, A2, and A3 obtained from thermogravimetric analysis (TGA), which was performed in air at a heating rate of 20 °C / min. The graphs illustrate the derivative of the sample's mass loss with respect to temperature.

[0045] Figure 20 This is a SEM micrograph of sample A2, which shows the encapsulated framework that appears to have broken and been damaged during processing.

[0046] Figure 21 Includes TEM micrographs of sample A2 at various magnifications. Figure 21 In A, the damaged encapsulated frame can be observed. Figure 21 In section B, a segment of the covering wall is shown. Figure 21 In section C, the graphite layers of the coated wall are shown. Dark stripes are outlined in yellow.

[0047] Figure 22 The single-point Raman spectrum of sample A2 is shown, obtained using a 532nm laser with a power setting of 2mW.

[0048] Figure 23 This is a SEM micrograph of compressed sample A1, showing the enveloped framework maintaining a three-dimensional macropore morphology with linear features in the wall due to buckling. A magnified inset shows the buckled wall.

[0049] Figure 24This is a SEM micrograph of compressed sample A2, showing the paper pattern assembly of a broken, flattened frame.

[0050] Figure 25 This is a SEM micrograph of the encapsulated framework in sample A3. Figure 25 A shows the polyhedral morphology of the encapsulated framework and the large, atomically flat facets. Figure 25 B shows a transparent window with a less transparent border. The two windows on the wall are circled and shaded in yellow. Figure 25 C indicates the concave curvature of the transparent window that extends across the border.

[0051] Figure 26 This is a SEM micrograph used to generate the polyhedral MgO template for sample A3.

[0052] Figure 27 Includes TEM micrographs of sample A3 at various magnifications. Figure 27 In diagram A, the cubic shape of the macroporous subunit of the encapsulated framework is shown. The edges of the cube are highlighted with yellow dashed lines. The more electron-transparent windows are highlighted with yellow solid lines. Figure 27 B shows a segment of the encapsulated wall. An enlarged illustration shows an example of a Y-dislocation found within the striations. Figure 27 C shows a wall of uniform thickness, even in the transparent "window" areas found within flat regions. This indicates that electron transparency is related to local sp. 3 The lack of state is related.

[0053] Figure 28 This shows a portion of the single-point Raman spectrum of sample A3. Features of interest are indicated by yellow circles. Features include the unfitted G band (G... u ), unfitted Tr features (Tr) u ), unfitted D-band (D u ) and 1100-1200cm -1 The unfitted shoulder between them. 1585cm -1 The conventional G peak position is marked with a dashed line, revealing the G peak position of sample A3. u Blue shift of the peak. The inset shows the full Raman spectrum of sample A3. The spectrum was acquired using a 532 nm laser with a power setting of 2 mW.

[0054] Figure 29 This is a diagram of the hypothetical zigzag geological interface formed between two ring-shaped disordered primordial domains (G1 and G2). The participating edge segments are labeled E1 and E2. The E1-E2 interface comprises three distinct interface zones—offset zone I, offset zone II, and horizontal zone. For ease of visual inspection, marked and unmarked vertical (V) and horizontal (H1 and H2) perspective views are shown. In the H2 perspective view, the highlighted yellow portion is set against the background.

[0055] Figure 30 The sp of the horizontal region across the E1-E2 interface is shown. 2 Grafting. The resulting sp 2 The rings form a ring connection between G1 and G2, resulting in a new graphene structure G3. For visual inspection, marked and unmarked vertical (V) and horizontal (H1 and H2) perspective views are shown. In perspective view H2, the highlighted yellow portion is set against the background.

[0056] Figure 31 The sp of the offset region across the E1-E2 interface is shown. 3 Grafting. New SP 2 Atoms are represented by black circles. New SP 3 Atoms are represented by black and white circles. The resulting sp x The rings include four rings (R1, R3, R5, R6) in a chair-like conformation, and two chiral rings (R1, R3, R5, R6) associated with the transition of the geological tectonic zone. 2-C R 4-C The chiral chains within the two chiral rings are indicated by blue arrows, and there are 5 sp... 3 -sp 3 The keys are indicated by red lines. The dotted reflection orientation of the chair-shaped ring and the two sp... are shown. 3 -sp 3 Key lines. Marked by sp across the offset region. 3 The grafting generates elevated tertiary free radicals. This is illustrated by the chiral ring R. 2-C The structure, in which its chiral ring is highlighted in blue, and its sp 3 -sp 3 The keys are highlighted in red. For visual inspection, marked and unmarked vertical (V) and horizontal (H1 and H2) perspective views are shown. In perspective view H2, the highlighted yellow portion is set against the background.

[0057] Figure 32 It is from Figure 32 Continuous z-direction growth occurs at the five elevated tertiary free radicals. New SP 3 Atoms are represented by black and white circles. The four rings (R1, R3, R5, R6) and two chiral rings (R...) are labeled in a chair conformation. 2-C R 4-C For ease of visual inspection, marked and unmarked vertical (V) and horizontal (H1 and H2) perspective views are shown. In perspective view H2, the highlighted portion is set against the background. This results in a second-level sp... 3 -sp 3 Keys are indicated by red lines. For visual inspection, marked and unmarked vertical (V) and horizontal (H1 and H2) perspective views are shown. In perspective view H2, the highlighted yellow portion is set against the background.

[0058] Figure 33 This is a diagram illustrating the continuous free radical addition above the basal layer. New SP 2 Atoms are represented by black circles. New SP 3 Atoms are represented as black and white circles. The three new sp atoms are labeled in a chair conformation. x Rings (R7, R8, R9) and two chiral rings (R 2-C R 4-C The sp, in a chair-like configuration x The addition of the ring produces two diamond-like carbon (DLC) seams, isolated as shown in the illustration of perspective view H1. These two DLC seams form the intersection of two Y-dislocations, as indicated by the shaded Y-shape in the illustration of perspective view H1. For visual inspection, marked and unmarked vertical (V) and horizontal (H1 and H2) perspective views are shown. In perspective view H2, the highlighted yellow portion is set against the background.

[0059] Figure 34 This is a diagram illustrating the continuous free radical addition above the basal layer. New sp 2 Atoms are represented by solid black circles, and the new sp 3 Atoms are represented by black and white circles. The third level of sp 3 -sp 3 The keys are highlighted in red. Three new SPs with a chair-like configuration have been marked. x Ring (R) 10 R 13 R 14 ) and 1 beginner sex ring (R 11-C Chiral ring R 11-C Located in chiral ring R 4-C Above this, chiral columns are formed. The chiral columns are shown isolated. Chiral chains 1 to 6 and 7 to 12 are indicated by blue arrows. For ease of visual inspection, marked and unmarked vertical (V) and horizontal (H1 and H2) perspective views are shown. In perspective view H2, the highlighted yellow portion is set against the background.

[0060] Figure 35 This is an illustration of the results of continuous radical addition above the basal layer. The rings above the basal layer have coalesced, and the second layer has nucleated. There are now four chiral rings (R...). 2-C R 4-C R 11-C R 12-C This creates two chiral columns. For visual inspection, marked and unmarked vertical (V) and horizontal (H1 and H2) perspective views are shown. In perspective view H2, the highlighted yellow portion is set against the background.

[0061] Figure 36This is an illustration of the continuous free radical addition above the basal layer. The third layer has already nucleated. One of the cubic diamond joints is highlighted in black in the enlarged inset. The other cubic diamond joint is highlighted in yellow in the second enlarged inset, and the chiral pillars representing the lateral ends of the joint are highlighted in blue (chiral chains) and red (z-direction sp). 3 -sp 3 (Chain). For ease of visual inspection, vertical (V) and horizontal (H1 and H2) perspective views are shown.

[0062] Figure 37 A is an enlarged view from the horizontal perspective view (H2), showing the chiral columns. Chiral chains within the chiral rings are highlighted in blue, while sp... (the connection between z and adjacent chiral rings) 3 -sp 3 The z-direction chain of the key is highlighted in red. Figure 37 In B, the chiral column structure is represented in a simplified graphical form. Figure 37 In C, sp within each chiral column x The spiral is isolated.

[0063] Figure 38 A is a SEM image of the C@MgO-coated composite particles unique to samples B1 to B3. MgO is observed as a bright charged region. Figure 38 In the SEM micrograph of sample B, the MgO template has been removed, leaving the unique encapsulation framework characteristic of samples B1 to B3. Figure 38 The SEM image of C shows the cell-sheet-coated framework unique to sample B4.

[0064] Figure 39 Raman spectra of samples B1-B4 are shown, and the observed spectral trends as temperature decreases are indicated.

[0065] Figure 40 This demonstrates how sp atoms can be produced in a boat-shaped conformation through interstitial atomic line grafting. x The zigzag-zigzag geological structure interface.

[0066] Figure 41 Showing the 5-yuan and 7-yuan sp x The zigzag-armchair geological structure interface formed by the grafting of two adjacent z-lines of the ring. These 5- and 7-membered rings are highlighted in yellow.

[0067] Figure 42 This demonstrates how sp atoms can be produced in a boat-shaped conformation through interstitial atomic line grafting. x The ring-shaped zigzag-armchair geological structure interface. These boat-shaped features are highlighted in yellow.

[0068] Figure 43This is a diagram illustrating the growth of multiple primordial domains on a common substrate surface, their grafting, and the nucleation and growth at higher levels. The "X" structures represent diamond-like carbon (DLC) joints. Some DLC joints propagate vertically, while others do not. New DLC joints are shown as being formed due to tectonic activity at higher levels.

[0069] Figure 44 It is the XRD line shape of sample B4.

[0070] Figure 45 These are images of samples C1 and C2, showing the degree of browning of these hydrogenated carbons.

[0071] Figure 46 This is the FTIR of sample C2. It indicates the hydrogenation of this brown coal sample.

[0072] Figure 47 These are the Raman spectra of samples C1 and C2. In each case, approximately 600 cm⁻¹ of the spectrum, attributed to the non-hydrogenated nanodiamond, was observed. -1 The secondary peak at this location indicates the non-hydrogenated phases of samples C1 and C2.

[0073] Figure 48 These are photographs of samples E1 and E1A of equivalent mass, showing the greater particle consistency of sample E1 and the finer, larger volume properties of sample E1A.

[0074] Figure 49 A to Figure 49 C is the SEM image of sample E1. Figure 49 D to Figure 49 F is the SEM image of sample E1A. Figure 49 A shows the particles of sample E1. (Compared to...) Figure 49 D, compared to sample E1A, indicates a more compact and granular representation of sample E1. Figure 49 B shows the flexibility of the wrapping frame and the curvature of the tissue paper sample in sample E1. Figure 49 E, compared to sample E1A, indicates the greater stiffness of the enclosing frame of sample E1A. Figure 49 C illustrates the fuzzy substructure of the encapsulated frame in sample E1. (And...) Figure 49 F, compared to sample E1A, indicates a more pronounced substructure within the rigid sample E1A frame.

[0075] Figure 50 A to Figure 50 C is the SEM image of sample E2. Figure 50 D to Figure 50 F is the SEM image of sample E2A. Figure 50 A shows the particles of sample E2. (Compared to...) Figure 50 D, compared to sample E2A, indicates a greater degree of densification and granularity in sample E2. Figure 50 B shows the flexibility of the wrapping frame and the curvature of the tissue paper sample in sample E2. (Compared to...) Figure 50 E, compared to sample E2A, indicates the greater stiffness of the enclosing frame of sample E2A. Figure 50 C illustrates the fuzzy substructure of the encapsulated frame in sample E2. (Compared to...) Figure 50 F, compared to sample E2A, indicates a more pronounced substructure within the rigid sample E2A frame. Sample E2A also indicates the fusion of the stacked plates.

[0076] Figures 51A and 51B are SEM images of the MgO template used to generate the granular framework used in Study E.

[0077] Figure 52 Showing sp x Raman spectral effects associated with precursor maturation.

[0078] Figure 53 This demonstrates the maturity-induced disintegration of a monolithic structure including cubic diamond-like seams.

[0079] Figure 54 This illustrates the role of chiral rings and chiral columns in maintaining vertical crosslinking during maturation.

[0080] Figure 55 It shows sp x spiral to sp 2 A diagram illustrating the transformation of a spiral.

[0081] Figure 56 It shows sp 2 Spirals around sp 2 A diagram illustrating the formation of a spiral.

[0082] Figure 57 Show Figure 36 sp x Maturation from precursor to helical monomer.

[0083] Figure 58 Provides enhancement for visual discrimination Figure 57 Another perspective view of the ring connectivity of the helical monomer shown.

[0084] Figure 59 It is the XRD line shape of sample B4A.

[0085] Figure 60 An alternative case is shown where the edges of G1 and G2 do not cross-intersect at the E1-E2 interface. It has been shown that in this case, the chiral ring R... 2-C and R 4-C It has opposite chirality, as indicated by the blue arrow.

[0086] Figure 61 Show spx Precursors in E1-E2 C Gradual growth above geological tectonic interfaces is reflected in Figure 29 The E1-E2 interface is modeled in the middle, but assuming sp 2 Grafting is not possible, and instead of the horizontal region, the E1-E2 interface includes the intersection point.

[0087] Figure 62 Showing through Figure 61 E1-E2 C sp constructed above geological tectonic interfaces x The double helix is ​​formed by the disintegration of the precursor.

[0088] Figure 63 The display is due to the span between E1 and E2 C sp formed by geological tectonic interfaces 3 -sp 3 The uncoupling of the bond lines leads to the complete uncoupling of the basal layer. Chiral ring R 3-C The two chiral chains in the diagram are indicated by blue arrows, sp 3 -sp 3 The keys are highlighted in red. Chiral chains are shown as point reflections. Sp 2 Atoms are indicated by black circles, while sp 3 Atoms are indicated by black and white circles.

[0089] Figure 64 Shown Figure 62 The formation of double helix modeled in the model and Figure 61 In E1-E2 C sp constructed above geological tectonic interfaces x Maturation-induced disintegration of the precursor. In R 3-C The chiral column constructed above is shown to contain sp x The double helix transforms into sp upon maturity. 2 Double helix.

[0090] Figure 65 Show horizontal areas and associated sp 2 How the absence or presence of grafts affects the loop connectivity of the resulting helical system.

[0091] Figure 66 Individual spirochetes and combined spirochetes are shown, including combined spirochetes with both common and opposite chirality.

[0092] Figure 67 This illustrates how a monolayer precursor can form a non-interlocking truncated double helix if it disintegrates during maturation.

[0093] Figure 68This illustrates how a bilayer precursor, if it disintegrates during maturation, forms sufficiently long double helices to interlock.

[0094] Figure 69 A is the graphical representation of the process from monomer to monomer maturity. Figure 69 B is the graphical theoretical representation of the transformation from a single entity to a composite.

[0095] Figure 70 This illustrates how two higher-level pathways extending upwards from the basal layer can reconnect to form a closed loop.

[0096] Figure 71 A shows the result from annealing sp x The precursor has a large-pore encapsulated frame. Figure 71 B shows a cross-section of the coated wall. The stripes exhibit a unique "slice" pattern, as indicated by the yellow lines, corresponding to a z-displacement of the helical graphene lattice around the dislocation lines for every 180° rotation. Figure 71 In C, the spirochete stretches across more than 10 layers of the helical network, as indicated by the yellow dashed guide line. Figure 71 In D, the combined helical loops originating from the unit cell wall are magnified. Through analysis... Figure 71 In the HRTEM image in D, we can see that the sp at the center of these two closely spaced helices... 2 The helical spacing is less than 1 nm.

[0097] Figure 72 A illustrates a helical x-network comprising a wrapped framework with an isometric cubic morphology. Figure 72 In diagram B, a controlled mesopore architecture of the coated frame is shown, exhibiting a highly consistent coated wall thickness. Figure 72 In B, the coated wall is shown at a higher magnification. It has an average of 2 to 3 layers and appears more twisted than a thicker wall due to its increased flexibility.

[0098] Figure 73 This is an illustration of three encapsulated frameworks demonstrating the concept of mesoscale crosslinking. The cross-hatching of structures I, II, and III indicates that their molecular-scale crosslinking is identical. However, their mesoscale crosslinking differs, with I exhibiting the highest level of mesoscale crosslinking and III the lowest.

[0099] Figure 74 A is a diagram of the hydroxylated edge formed by the vertical ends of two combined helices. Figure 74 B is a diagram representing an entrance to the interlayered labyrinth of the network. These entrances provide ubiquitous entry points for the seepage or expulsion of liquids, such as... Figure 74 As shown in B.

[0100] Figure 75These are a series of SEM micrographs of the fractured surface of an epoxy nanocomposite. The nanocomposite comprises 0.5% by weight of sp... x Network. Each embedded encapsulated framework includes a cell-layer morphology (e.g., Figure 75 (indicated by the yellow circle in C) and sp x network.

[0101] Figure 76 These are a series of SEM micrographs of the fractured surface of the epoxy nanocomposite material. The surface is covered with debris generated by the explosive fracture of the cured epoxy nanocomposite material near the coated framework. Figure 76 In section B, we can see a result of such an explosion and rupture. Figure 76 In C, we can observe that the debris is epoxy resin fragments physically embedded in the surface.

[0102] Figure 77 There are two sps x The networks are compressed together to form a non-native bilayer that can be crosslinked during maturation.

[0103] Figure 78 These are two sps in static VdW contact. x Network G A With G B A diagram illustrating the free radical addition reaction between G and G. This is shown in image I. The geometry of the underlying helix will... B sp 2 Free radicals toward G A Promote, such as Figure 78 As shown in image II, free radicals are circled. The free radical cascade reaction will... B sp 2 Free baseline and G A The z-adjacent atoms in the matrix bond together, thus forming sp. 2 Ring. This reaction causes the spirochete to extend across the non-native bilayer, such as... Figure 78 As shown in picture III, it pushes the edge dislocations terminated by free radicals toward the surface.

[0104] Figure 79 A is sample particle F1. Figure 79 B is sample F2 fragment.

[0105] Figure 80 shows the N2 adsorption isotherms for samples F1-F4.

[0106] Figure 81 This is a pore distribution chart for samples F1-F4.

[0107] Figure 82 These are the Raman spectra of samples F1-F4.

[0108] Figure 83 The Raman spectral changes associated with the maturation of sample F2 granules into sample F3 are shown.

[0109] Figure 84 A is a photo of Buck paper. Figure 84 B is a picture of a piece of Buck paper.

[0110] Figure 85 A is a SEM micrograph of a cross-section of Buck paper. Figure 85 B shows the collapsed wrapping frame that makes up the Buck paper. Figure 85 C shows the K2CO3 template.

[0111] Figure 86 This is a solvent impregnation test on unannealed Buck paper.

[0112] Figure 87 This is a solvent impregnation test on unannealed Buck paper.

[0113] Figure 88 These are the Raman spectra of samples F5 and F6.

[0114] Figure 89 It is composed of slender sp x Fiber-like Buck paper made from macroscopic materials.

[0115] Figure 90 A is a SEM image showing fibrous Buck paper. Figure 90 B shows a flexible, slender sp x microstructures .

[0116] Figure 91 It is a SEM micrograph of a finely compact encapsulated framework with fuzzy substructure features.

[0117] Figure 92 It is a SEM micrograph of a rough, non-compact frame.

[0118] Figure 93 This is a SEM micrograph of a petal-shaped framework.

[0119] Figure 94 These are SEM micrographs of two hollow spherical frameworks.

[0120] Figure 95 These are SEM micrographs of two isometric frames.

[0121] Figure 96 This is a photograph of sample G1, which has undergone resistance heating at 1 atmosphere.

[0122] Figure 97 This is a sequence of photographs showing sample G1 exhibiting the Meissner effect.

[0123] Figure 98 These are photographs of various disordered carbon samples subjected to resistance heating at 1 atmosphere of pressure.

[0124] Figure 99 It is a photograph of a disordered carbon sample exhibiting the Meissner effect.

[0125] Figure 100 This is a photograph of a disordered carbon sample exhibiting flux pinning in the presence of neodymium magnets.

[0126] Figure 101 A is a TEM micrograph showing a typical encapsulated framework in sample G1. Figure 101 B is the XRD line shape of sample G1. Figure 101 C is the Raman spectrum of sample G1.

[0127] Figure 102 It shows sp x The sp network grows around the surface of the underlying template until completion. x A layered model. This can be considered a sp. x The cross-section of the network.

[0128] Figure 103 A is a photograph of the granular MgO template used in the study of H. Figure 103 B is a photograph of a porous coated composite material formed on MgO flakes.

[0129] Figure 104 These are photographs showing the contact between the four probes in H and the coated composite material.

[0130] Figure 105 It is a graph that studies the effect of the sheet resistance of the sample in H on the chamber pressure.

[0131] Figure 106 This is the Raman spectrum of the sample used in study H. The Raman spectrum did not change after the tests performed in study H.

[0132] Figure 107 This is a schematic diagram illustrating a method for forming environmentally superconducting products, such as filaments, by venting internal gases, applying an impermeable barrier phase, and then restoring the product to external environmental pressure.

[0133] Figure 108 This is a photograph of the probe tip, showing the molten area of ​​the plastic casing where the probe tip heats up. The molten area is circled.

[0134] Figure 109 A is an HR-TEM image of the enveloped frame including BN. Figure 109 B shows the Y-dislocation that exists through the envelope wall. Figure 109 C shows a screw dislocation that also exists throughout the envelope wall. Detailed Implementation

[0135] This chapter is organized according to the following outline:

[0136] I. Basic Terminology and Concepts

[0137] We provide basic definitions and establish fundamental concepts for describing structures.

[0138] II. Surface Replication

[0139] We introduce fundamental concepts related to template making, and particularly to surface replication. These concepts are more comprehensively understood in applications '918 and '760.

[0140] III. Free Radical Cryopolymer Growth and Geological Structure

[0141] We discuss how graphene networks nucleate and grow into radical condensates. We also discuss the geological interactions between graphene domains during growth.

[0142] IV. Surfaces in Three Dimensions

[0143] We discuss curved surfaces and establish certain conventions to guide ourselves when discussing complex structures in three-dimensional space.

[0144] V. Clarify the example

[0145] We analyze and discuss exemplary structures in order to clarify definitions and basic concepts.

[0146] VI. Notes on Metrology and Characterization

[0147] We provide details about the metrology used in this disclosure and discuss the Raman spectral characteristics of disordered carbon.

[0148] VII. Procedure

[0149] We explain the detailed procedures used to synthesize the carbon samples for experiments A through G.

[0150] VIII. Study A—Analysis

[0151] Study A includes: (i) the synthesis of synthetic anthracite networks; (ii) sp x Network synthesis; (ii)sp 2 and sp 3个 Modeling of grafting; (iii) Modeling of diamond-like joints and chiral column formation; (iv) Modeling of multilayer growth; and (v) Discussion of free radical condensates.

[0152] IX. Study B—Analysis

[0153] Study B includes: (i)spx and x-sp x (ii) Network synthesis; (iii) Modeling of various geological structural interfaces; (iv) Post-hoc analysis and discussion of the limitations of existing technologies.

[0154] X. Research C—Analysis

[0155] Study C includes: (i) demonstration of incomplete dehydrogenation during the growth of free radical condensates; and (ii) spectroscopic analysis of the hydrogenated and dehydrogenated carbon phases.

[0156] XI. Research D—Analysis

[0157] Study D includes demonstrations of improved grafting by adding hydrogen during the growth of free radical condensates.

[0158] XII. Research E-analysis

[0159] Research E includes: (i)x-sp x Network and z-sp x (i) Maturation of mature x-networks and mature z-networks; (ii) Modeling of structural changes during maturation; (iii) Analysis of mature networks.

[0160] XIII. Study F—Analysis and Discussion

[0161] Study F includes: (i) a demonstration of particle-to-particle crosslinks through maturation; (ii) a demonstration of macroscopic lamellar and blocky forms of mature x and z networks; and (iii) a discussion of crosslinks through maturation.

[0162] XIV. Study G – Analysis and Discussion

[0163] Study G includes: (i) demonstration of microwave-induced resistance heating; (ii) demonstration of diamagnetism and room-temperature superconductivity in anthracite networks synthesized under reduced pressure; (iii) demonstration of diamagnetism and room-temperature superconductivity in other disordered pyrolytic carbons under reduced pressure; and (iv) discussion of the theoretical basis of the observations.

[0164] XV. Study H—Analysis and Discussion

[0165] Study H includes: (i) demonstration of environmental superconductivity in macroscopic volumes of evacuated anthracite; and (ii) discussion of the theoretical basis of the observation.

[0166] XVI. Other Anthracite Networks

[0167] Our discussion includes BN and BC. x Synthesis of anthracite network from non-carbon chemical compositions of N.

[0168] I. Basic Terminology and Concepts

[0169] As used in this article, the term "graphene" describes sp 2 Hybrid atoms or sp 3 Two-dimensional polycyclic structures of hybrid atoms. Although graphene represents a form of carbon, we use the term "graphene-like" in this paper to describe a variety of graphene polymorphs (including known or theoretical polymorphs such as graphene, amorphous graphene, phane graphene, Haeckel carbon, etc.), as well as other two-dimensional graphene analogues (e.g., BN, BC). x (N, etc., an atomic monolayer). Therefore, the term "graphene" is intended to encompass those satisfying two-dimensional polycyclic structures and sp. 2 or sp 3 Any assumption of the basic criteria for hybridization of polymorphs.

[0170] The term "two-dimensional" in this article refers to molecular-scale structures at the level of a single layer of atoms. Two-dimensional structures can be embedded or immersed in higher-dimensional spaces to form larger-scale structures, at which point the structure can be described as three-dimensional. For example, a sub-nanometer-thick graphene lattice may be bent in three-dimensional space to form atomically thin walls of a nanoscale three-dimensional unit cell. This unit cell will still be described as two-dimensional at the molecular scale.

[0171] A “ring” is defined herein as a covalent chain of atoms that together form a closed polyatomic polygon with fewer than 10 atomic vertices. Each of the ring structures in a polycyclic layout comprises a ring. Each of the atoms constituting a given ring can be described as an atomic member belonging to that ring, and the ring can be described accordingly (i.e., a “6-membered” ring describes a hexagonal ring formed by 6 atomic members).

[0172] sp 2 In this paper, a "ring" is defined as a ring whose atomic members are all sp. 2 Rings of hybrid atomic members.

[0173] sp x In this paper, a "ring" is defined as a ring in which not all of the included atomic members share the same orbital hybridization.

[0174] A “chiral ring” is defined in this paper as a covalent chain in which the atomic members comprise one or more chiral segments. x Rings, in which the two atomic ends of these chiral segments are connected by sp... 3 -sp 3 sp keys connected to each other 3 Hybrid atoms. Chiral rings appear at the transition zones of geological structures.

[0175] In this paper, a "chiral column" is defined as a column formed by sp... 3 -sp 3A chiral pillar is a series of z-adjacent chiral rings interconnected by one or more z-direction chains of a bond. Chiral pillars typically form above the basal layer chiral rings and represent the lateral ends of diamond-like carbon (DLC) seams. A chiral pillar may contain one or more sp... x spiral.

[0176] sp x "Helix" is defined in this paper as being composed of sp 2 Hybridized atomic members and sp 3 A helical one-dimensional chain constructed by two hybrid atomic members. x The axis of the helix is ​​z-oriented.

[0177] sp x The "double helix" is defined in this paper as consisting of two sp1 cells sharing the same chirality and the same axis. x A spiral structure.

[0178] sp 2 "Helix" is defined in this paper as being composed of only sp 2 A helical one-dimensional chain constructed from hybrid atomic members. x The axis of the helix is ​​z-oriented.

[0179] sp 2 The "double helix" is defined in this paper as consisting of two sp1 cells sharing the same chirality and the same axis. 2 A spiral structure.

[0180] "Adjacent rings" in this document describe two rings that have at least two common atomic members and therefore share at least one common edge. In organic chemistry, these rings may include fused rings or bridged rings, but not spirorings. Two adjacent rings may be described as "ring-adjacent".

[0181] The term "ring-connected" in this paper describes structures connected by "ring pathways" or paths between adjacent rings. We can discuss ring connectivity in two ways. In the first usage, we can say that one part of the structure is ring-connected to another part of the structure. This means that there exists a ring pathway connecting the two mentioned parts. For example, if there is a path between adjacent rings that start at ring R1 within the graphene structure and end at another ring R2 within the structure, then ring R1 is connected to ring R2. In the second usage, we can say that the mentioned structure itself is ring-connected. This means that any part of the mentioned structure can be reached from any other part through at least one ring pathway. We can also describe non-ring-connected structures as having disconnected rings.

[0182] The term "loop pathway" in this paper describes a pathway connecting two mentioned structures to adjacent loops.

[0183] The term "ring connection" in this paper describes a ring connection between two single rings of the mentioned structures.

[0184] “Sp 2 The ring connection described in this article is via "sp". 2 "Loop path" or adjacent sp 2 The structure of path connections in a ring. Similar to ring connectivity, we can discuss sp in two ways. 2 Ring connectivity. In the first usage, we can say that a part of the structure is sp. 2 The ring connects to another part of the structure. This means there exists a sp that connects the two mentioned parts. 2 Loop pathway. In the second usage, we can say that the structure mentioned itself is sp. 2 The ring connection means that any part of the mentioned structure can be connected via at least one sp. 2 The loop path arrives from any other part. Because of sp 2 Ring connectivity is a specific case of ring connectivity, therefore it implies ring connectivity, while ring connectivity does not imply sp. 2 Ring connectivity. In some cases, we can describe certain ring-connected structures as "sp". 2 "The loop is broken" means that although they are connected in a loop, they are not connected via sp. 2 The loop path is connected in a loop.

[0185] An “edge atom” is defined as an atom that (i) belongs to a ring and (ii) is not surrounded by a ring on all four sides. Edge atoms always have multiple nearest neighbors that are also edge atoms, thus forming a chain.

[0186] An “edge” is defined as a chain of edge atoms. Starting from any given edge atom, a chain of nearest-neighbor edge atoms can be traced from that first atom, where any given pair of nearest-neighbor edge atoms within the chain is a co-member of exactly one loop. Some edges can form closed loops, where the first and last atoms traced are each other’s nearest neighbors.

[0187] An “edge segment” is defined as a chain of nearest-neighbor edge atoms contained within a larger edge.

[0188] "Internal atom" is defined in this paper as (i) an atom that belongs to a ring and (ii) is surrounded by a ring on all four sides.

[0189] In this paper, a "graphene structure" is defined as a polycyclic ring linker consisting of two or more rings. Each ring in a graphene structure is linked to every other ring, but not necessarily sp. 2 The atoms are ring-connected. Each atom in the graphene structure can be classified as an inner atom or an edge atom.

[0190] In this paper, a “graphene region” or “region” is defined as an accessory part of a larger graphene structure that satisfies all the requirements of a graphene structure.

[0191] “Cyclic disorder” is defined in this paper as the presence of non-hexagonal rings in a graphene structure. Cyclic disordered graphene structures include amorphous, Haeckel carbon, pentagonal, or other molecular splicing. The presence of non-hexagonal rings creates regions of non-zero Gaussian curvature in cyclic disordered graphene structures. If inserted into a hexagonal splice lattice, a 5-membered ring exhibits positive Gaussian curvature, while a 7-membered ring induces negative Gaussian curvature. For example, fullerenes comprise curved graphene structures formed by 20 hexagons and 12 pentagons.

[0192] “Ring order” is defined in this paper as essentially a hexagonal molecular assembly. Ring-ordered graphene structures can bend or wrinkle due to their low bending stiffness.

[0193] "System" is defined herein as a multi-atom physical structure comprising a group of atoms cohesively bound together by chemical bonds or van der Waals interactions. A system may contain any number of graphene structures, including those without graphene. It is a general term used to describe a particular physical structure under consideration.

[0194] In this paper, a “graphene system” is defined as a system consisting of one or more different graphene structures. Graphene structures belonging to a graphene system can be described as “graphene members” or “members” of the graphene system. A graphene system does not include any elements other than its graphene members.

[0195] "Graphene monomer" or "monomer" is defined in this paper as a graphene system comprising a single graphene structure of different types.

[0196] "Graphene assembly" or "assembly" is defined herein as a graphene system comprising two or more different graphene structures.

[0197] "Van der Waals" or "vdW assemblies" are defined in this paper as multilayer graphene assemblies in which the graphene structures are primarily or substantially cohesive through intermolecular forces. The graphene structures in vdW assemblies can also be cohesive through other mechanisms.

[0198] In this paper, a "double-screw dislocation" is defined as a dislocation formed by two screw dislocations sharing the same chirality and the same dislocation line. Double-screw dislocations in graphene systems form graphene double helices. The braided geometry of the double helix physically interlocks the two helices.

[0199] In this paper, a “multilayer” graphene system is defined as a graphene system with more than one layer on average, including vdW contacts. Multilayer graphene systems can have monolayer regions. Analytically, we can define a multilayer graphene system as having a region not exceeding 2,300 m², as measured by N₂ adsorption. 2 The system with an average BET surface area of ​​ / g.

[0200] In this paper, "Y-dislocations" are defined as Y-shaped graphene regions formed by layer bifurcation into rings connected laterally adjacent bilayers. The two "branches" of the Y-shaped region include z-adjacent sp... x The rings together form a diamond-like carbon (DLC) joint at the interface between laterally adjacent layers and the double layer. The characteristic Y-shaped geometry is associated with the cross-sectional plane of the layer and the DLC joint.

[0201] In this paper, a "diamond-like joint" or "joint" is defined as a z-adjacent spline forming a z-oriented interface between two xy-oriented layers. x Two-dimensional layers of rings. Cubic diamond-like joints include chair conformations, while hexagonal diamond-like joints include chair, boat, and possibly other conformations. Diamond-like joints may terminate at chiral pillars.

[0202] A “bond line” is a linear arrangement of two or more side-by-side bonds with a generally parallel (but not necessarily perfectly parallel) orientation.

[0203] The term "graphene network" in this paper describes a structure with a two-dimensional molecular-scale geometry that is three-dimensionally cross-linked at a larger scale. Based on the cross-linking and network geometry of graphene networks, they cannot be destroyed without disrupting a portion of their two-dimensional molecular structure. Graphene networks encompass the broadest category of networks constructed from graphene structures, such as... Figure 1 The location of the vertex in the classification chart is shown. The requirement for three-dimensional crosslinking at certain evaluation scales excludes graphene systems (such as simple polycyclic aromatic hydrocarbons) that cannot be called three-dimensionally crosslinked at any scale, as defined here. In this disclosure, the term "graphene network" follows our use of the term "of graphene," as it will generally be used to apply to networks of two-dimensional molecular structures, including a wide variety of polymorphs and chemicals. In the specific case of carbon graphene networks, we can further describe the network in terms of the anisotropy of molecular-scale crosslinking:

[0204] ●“Highly anisotropic”, if the average I 2Du / I Gu The ratio is higher than 0.40

[0205] ●“Moderately anisotropic”, if the average I 2Du / I Gu The ratio is between 0.20 and 0.40.

[0206] ●“Minimal anisotropy”, if the average I 2Du / I Gu The ratio is less than 0.20

[0207] In this paper, a "layered" network is defined as a multilayer graphene network comprising z-adjacent layers of graphite or nematic xy arrangement. Layered graphene networks in... Figure 1 The classification chart shows it as a subcategory of graphene networks. As shown in Figure 2, the Schwarz structure does not include a layered graphene network.

[0208] In this paper, a “graphite network” is defined as a hierarchical graphene network in which z-adjacent layers exhibit a graphite xy arrangement (i.e., they are substantially parallel). The characteristics of a graphite network are... or smaller average <002> The interlayer spacing d does not exist in large quantities greater than The interlayer spacing of graphite networks. Figure 1 The classification chart shows it as a subcategory of layered graphene networks.

[0209] The term "anthracite network" is defined herein as a hierarchical graphene network comprising a two-dimensional molecular structure cross-linked by certain characteristic structural dislocations described herein as "anthracite dislocations," including Y-dislocations, screw dislocations, and mixed dislocations exhibiting characteristics of both Y-dislocations and screw dislocations. The z-adjacent layers in the anthracite network exhibit a nematic arrangement. The anthracite network is characterized by a large number of layers larger than […]. of <002> Interlayer spacing d. Anthracite network in Figure 1 The classification chart shows them as subcategories of graphene networks, and they can be further classified into natural (i.e., anthracite) and synthetic, with synthetic anthracite networks being more diverse in terms of architecture and chemistry.

[0210] The term "nematic arrangement" is used in this paper to describe the molecular-scale general xy arrangement between z-adjacent layers in a multilayer graphene system. This term is commonly used to refer to a uniform but incomplete xy arrangement observed between liquid crystal layers, and we find it applicable in this paper to describe the incomplete xy arrangement of z-adjacent layers in anthracite networks. Nematic arrangements are characterized by a large number of molecules larger than […]. of <002> Interlayer spacing d.

[0211] sp x In this paper, "network" is defined as a synthetic anthracite network comprising a single continuous graphene structure, wherein the network is cross-linked laterally and vertically via diamond-like seams and mixed dislocations (e.g., chiral pillars). In the context of the maturation process, sp... x A network can be described as "sp x "Precursor".

[0212] carbon sp x Networks can be further classified based on the degree of their internal grafting, which can be determined by their sp. size before maturity. 2 The prevalence of hybridized edge states is used to determine this. Regarding the degree of this grafting, carbon sp... x A network can be described as:

[0213] ●“Very few grafts”, if (a) its average D u The position is located at 1342cm -1 Above, (b) its average D f The peak is located at 1342cm. -1 Below, and (c) no point spectrum shows below 1342 cm⁻¹ -1 D u Peak

[0214] ●“Partial grafting”, if (a) its average D u The peak is located at 1332cm. -1 With 1342cm -1 Between, and (b) no point spectrum shows below 1332 cm⁻¹ -1 D u Peak position; or alternatively, if (a) its average D u The peak is located at 1342cm. -1 Above, and point (b) shows a spectrum between 1332 cm⁻¹ -1 With 1340cm -1 Between D u Peak position.

[0215] ●“High-level grafting”, if its average D u The peak is located at 1332cm. -1 Above; or alternatively, (a) its average D u The peak is located at 1332cm. -1 Above, and (b) some point spectra show below 1332 cm⁻¹ -1 Local D u Peak position.

[0216] These conditions are summarized in Table 1 below:

[0217] Table 1

[0218]

[0219]

[0220] The term "spiral network" is defined in this paper as a synthetic anthracite network comprising spiral dislocations. These spiral dislocations can be generated through the presence of sp xThe maturation and formation of chiral pillars in the network. Therefore, sp x The network can be described as a "sp" of a spiral network. x "Precursor". Helical network from sp x Precursor derivation Figure 1 The classification chart is indicated by a dashed line labeled "mature".

[0221] "Maturity" in this article is defined as the process accompanying sp. x sp in the precursor 3 sp in hybrid state 3 to sp 2 Rehybridization structural transformation. x The maturation of the precursor eventually forms a helical network; the degree of maturity is determined by sp. 3 to sp 2 The degree of completion of rehybridization is determined. Maturation is gradual, therefore it can form processes including sp. x A network that is somewhere between a spiral network and a helical network. Furthermore, maturation can be localized; for example, heating certain locations within the network (such as via a laser) may induce localized maturation in the affected area.

[0222] In this paper, a “highly mature” carbon helical network is defined as having a diameter of at least 1340 cm⁻¹. -1 And compared to its sp x The forebody height is at least 8cm -1 Average D u The carbon helical network at the peak position.

[0223] In this paper, “x-carbon” is defined as a class of synthetic anthracite networks constructed from graphene and including one of the following:

[0224] ●"x-sp" x "Network" is defined in this article as a highly grafted sp x network

[0225] ●“Helical X-carbon,” by making x-sp x Precursor maturation to intermediate or highly mature state is formed

[0226] In this paper, “z-carbon” is defined as a class of synthetic anthracite networks constructed from graphene and including one of the following:

[0227] ●“z-sp x "Network" is defined as a network with very few or no grafted sp. x network

[0228] ●“Helical Z-carbon,” achieved by making z-sp x Precursor maturation to intermediate or highly mature state is formed

[0229] When used in the context of identifying z-carbons, the z-prefix is ​​independent of z-directivity.

[0230] "Helical monomer" is defined in this paper as a monomeric helical network, wherein the helical network comprises a single ring connecting a graphene structure, and wherein the network is cross-linked laterally and vertically by helical dislocations.

[0231] "Helical assemblages" are defined in this paper as assemblages of helical networks, which consist of assemblages of multiple helical graphene structures physically interlocked with each other by braided double helices (i.e., double helical dislocations).

[0232] sp x "Prefabricated body" is a different sp x The precursor (referred to as "sp" in this context) x A macroscopic composite of microscopic entities. Various molding techniques can be used to give sp... x The desired shape of the preform is such as slender, flat, or equiaxial.

[0233] In this paper, "macrobody" is defined as macro-cohesive structure.

[0234] "Monomer-to-monomer" maturation is defined in this paper as sp. x The maturation process of precursor maturation to form helical monomers.

[0235] The maturity of "from single entity to composite" is defined in this paper as the sp... x The maturation process of precursors disintegrating into helical assemblages.

[0236] "Disintegration" is defined in this paper as the breaking apart of a monomeric graphene network into two or more distinct rings, thus breaking the graphene structure.

[0237] “Primitive domains” are defined in this paper as graphene domains that nucleate and grow on a substrate before encountering any geological formations. When primitive domains grow toward each other on a common surface, their edges may have geological formations encountering each other.

[0238] In this paper, the "primitive region" is defined as the region of a graphene network that roughly coincides with the network's original domain. We typically refer to the primitive region when the initial description of a graphene system is of a region within the original domain.

[0239] "Geological tectonic encounter" is a state of lateral close contact between two edge segments during the growth of a two-dimensional lattice. A geological tectonic encounter forms a geological tectonic interface between two participating edge segments. Numerous geological tectonic encounters that can occur during the nucleation and growth of graphene systems can be described as "geological tectonic activity."

[0240] In this paper, “geological structural interface” is defined as an edge-to-edge interface formed by the encounter of geological structures between two graphene structures or regions.

[0241] In this paper, a “Z-shaped-Z-shaped interface” is defined as a geological tectonic interface in which two edge segments are located in a Z-shaped configuration.

[0242] The “zigzag-armchair interface” is defined in this paper as a geological tectonic interface in which one of the edge segments is in a zigzag configuration and the other is in an armchair configuration.

[0243] The term “offset zone” is defined in this paper as an interface zone within a geological tectonic interface, in which one of two participating edge segments is vertically offset, i.e., one edge segment is located above the other.

[0244] In this paper, the term "horizontal zone" is defined as an interface zone within a geological tectonic boundary, in which two participating edge segments are substantially horizontal to each other and sufficiently aligned to form two or more laterally adjacent sps across the interface. 2 -sp 2 The bond line of the bond, thus generating one or more sps. 2 Ring connection.

[0245] In this paper, an "intersection" is defined as a location within a geological tectonic interface where two participating edge segments intersect at a cross and their arrangement is insufficient to form two or more laterally adjacent sps. 2 -sp 2 The key line. This may be due to the relative sp. 2 The two p atoms of the edge atom z The orbitals are too misaligned to form a π bond.

[0246] “Sp 2 "Grafting" is defined in this paper as sp between two edge atoms. 2 -sp 2 Bond line formation. Sp 2 Grafting can cause different graphene structural rings to connect and aggregate into larger graphene structures. 2 Ring connection. SP across geological structural interfaces. 2 Grafting is advantageous in horizontal areas.

[0247] “Sp 3 "Grafting" is defined in this paper as sp between two edge atoms. 3 -sp 3 Bond formation. This may involve sp 2 sp of edge atoms 2 to sp 3 Rehybridization. Sp 3Grafting can cause different graphene structural rings to connect and aggregate into larger graphene structures. x Rings. SPs spanning geological tectonic interfaces. 3 Grafting is advantageous in the offset zone.

[0248] The “base” or “base layer” is defined in this paper as the first graphene layer formed by grafting across the geological tectonic interface between the original domains during pyrolysis growth.

[0249] The term “mesoscale” is used in this paper to describe a hierarchical level or characteristic (e.g., crosslinking, porosity) that relates to a size scale relatively larger than molecular features. For example, the mesoscale crosslinking of a coated framework varies with its crosslinking at a size scale that is more relevant to discussions of its particle morphology than to discussions of its molecular bonding structure.

[0250] Following IUPAC convention, "micropores" are defined in this paper as pores with a diameter of less than 2 nm. A "microporous" structure or phase is characterized by the presence of micropores.

[0251] Following IUPAC convention, "mesopore" is defined in this paper as a pore with a diameter between 2 nm and 50 nm. A "mesopore" structure or phase is characterized by the presence of mesopores.

[0252] Following IUPAC convention, "macropores" are defined in this paper as pores with a diameter greater than 50 nm. Macropore structures or phases are characterized by the presence of large pores.

[0253] "Environmental superconductor" is defined in this paper as a material or article capable of entering a superconducting state at a temperature above 0°C and an external pressure of 0 to 2 atmospheres. "Environmental superconductivity" is defined in this paper as the superconducting state at a temperature above 0°C and an external pressure of 0 to 2 atmospheres.

[0254] II. Surface Replication

[0255] Pyrolysis involves the decomposition of gaseous, liquid, or solid carbonaceous materials and can be used to form graphene structures. In some pyrolysis procedures, this decomposition occurs on a substrate surface. The substrate can include a simple flat foil surface or a more complex particle surface. Graphene systems synthesized on particles can inherit some of the particles' morphological properties. In our '918 and '760 applications, we defined several terms related to template-directed synthesis. These terms are defined below.

[0256] As defined in this paper, a “template” is a potential sacrificial structure that imparts a desired morphology to another material formed therein or on. Related to surface replication technology are the surface on which the template is positively replicated (i.e., the “template surface”) and the bulk phase on which it is negatively replicated (i.e., the “template body”). Templates can also play other roles, such as catalyzing the formation of coated materials. A “template-based” structure is a structure that replicates a feature of the template.

[0257] "Covered" or "covered" material is a material formed within or on top of a solid or "hard" template material.

[0258] As defined herein, “surface replication” includes template techniques in which the surface of a template is used to guide the formation of a thin coating wall of the adsorbed material, the wall substantially encapsulating and replicating the template surface formed thereon. Subsequently, upon displacement, the template body is negatively replicated by the intracellular space within the coating wall. Surface replication produces a coating framework with a templated pore wall architecture.

[0259] As defined herein, a “coated framework” (or “framework”) is a nanostructured coating formed during surface replication. A coated framework comprises nanostructured “coated walls” (or “walls”) with thicknesses ranging from less than 1 nm to 100 nm, but preferably between 0.6 nm and 5 nm. Because the coated walls essentially encapsulate and replicate the template surface, they can be described as “conformal.” Coated frameworks can be fabricated into diverse structures, ranging from simple hollow architectures formed on non-porous templates to labyrinthine architectures formed on porous templates. They can also comprise different chemical compositions. Typical frameworks can be constructed from carbon and may be referred to as “carbon-coated frameworks.”

[0260] As defined herein, “content” includes the template because it exists within a substantially enclosed envelope phase. Therefore, once an envelope phase has been formed around the template, the template can be described as content or “content-based.”

[0261] As defined herein, a “coated composite” is a composite structure comprising contents and a coating body. A coated composite can be represented as x@y, where x is the coating element or compound, and y is the content element or compound. For example, a coated composite comprising carbon coating bodies on MgO contents can be represented as C@MgO.

[0262] Numerous template elements or compounds can be used, including carbon, metal oxides, oxygen-containing anionic salts, boron nitride, metal halides, etc. In particular, magnesium oxide (MgO) templates are frequently used in chemical vapor deposition (“CVD”) processes due to their stability at high temperatures. Many of these templates are described in applications '918 and '154. All that is required for many surface replication procedures involved in CVD is the nucleation of the surface and the lattice, which can be grown either autocatalystly or as a free radical condensate.

[0263] III. Free Radical Cryopolymer Growth and Geological Structure

[0264] In the theory of radical condensate growth, radical condensates (i.e., "condensates" or "FRCs") form during the pyrolytic decomposition of reactive vapors. Carbon FRCs are charged hydrogenation precursors to graphene structures, capable of rapidly rearranging their carbon skeletons without breaking covalent bonds; thus, they can be considered as charged covalent liquids. Carbon FRCs grow via radical addition reactions at their edges in the presence of reactive vapors. As the condensate releases molecular hydrogen, its radical concentration decreases, its self-rearrangement ceases, and it becomes an uncharged carbon structure. The gradual release of molecular hydrogen provides the FRC with more time to rearrange itself into an energy-minimizing configuration—typically one that eliminates high-energy edge defects. This has been shown to contribute to edgeless graphene structures, such as fullerenes. In contrast, the sudden loss of hydrogen does not provide sufficient time for these energy-minimizing rearrangements to occur, which promotes the formation of graphene structures with more edges.

[0265] If grown on a common substrate surface, graphene structures can make lateral contact with each other. The encounters of these geological formations and the potential factors determining how they resolve have been a subject of little research. In one instance, researchers observing the growth of ring-ordered crystalline graphene structures on copper foil discovered that geological formations can encounter each other in one of two ways (e.g., Figure 5 (As shown in A) Solution.

[0266] In the first scenario, one edge of the graphene structure is subducted by the edge of another—an event described herein as a "subduction event." Subduction events allow the subducted region to continue growing on top of the subducted region, such as... Figure 5 As shown in B. The continued growth of the subduction zone is due to... Figure 5 The black arrow in B indicates that growth in the subducted area is suppressed, such as... Figure 5 As shown in B, the subduction event forms edge dislocations in two overlapping z-adjacent graphene structures that are weakly cohesive through van der Waals interactions.

[0267] In the second scenario described by the researchers, one edge of the graphene structure can be connected via sp_t between opposing edge atoms.2 -sp 2 Bonds are formed and grafted to the edge of another. This sp 2 Grafting causes two graphene structures to coalesce into a larger graphene structure. The result of this event is... Figure 5 As shown in C. Researchers have shown that sp between lateral or rotational misaligned edges 2 Grafting can lead to the formation of non-hexagonal rings in the new graphene structure. Therefore, sp 2 The regional presence of these non-hexagonal rings within the grafted domain can induce local lattice curvature, such as... Figure 5 As shown in C.

[0268] The complexity of the geological structures between graphene structures increases as the substrate surface becomes more topologically and morphologically complex. This complexity increases further if we assume edge disorder. We speculate here that these factors are important in determining the outcome of geological structure encounters. Finally, complexity increases if the geological structures occur in essentially unconstrained spaces where the spatial effects of surrounding structures are negligible. This is not the case when pyrolysis occurs in certain microporous template particles (such as zeolite Y), where sp. inter-structure interactions between graphene structures may be forced due to z-direction constraints in the micropores of these templates (i.e., lack of top clearance). 2 Grafting (different from subduction).

[0269] IV. Surfaces in Three Dimensions

[0270] To describe the local space surrounding a curved two-dimensional graphene structure, it is helpful to establish an intuitive orientation. On a curved surface, there exists a plane at any given point, which we can consider as the xy plane. Figure 3 The hypothetical structure and the tangent plane highlighted in yellow at a certain point are shown. Consistent with this, the z-axis, orthogonal to this xy-plane, is also present. Figure 3 As shown in the diagram. Although the orientation of the tangential plane and the z-axis will vary across the curved surface, we find it helpful to describe the local space roughly above or below the graphene region as "z-space" and the orientation of the local z-space as "vertical". We also find it helpful to describe the direction perpendicular to the local z-axis as "lateral".

[0271] Examples of cyclic disordered graphene domains with non-zero curvature in Figure 4 Modeling was performed. This model was constructed using Avogadro 1.2.0 software and relaxed to obtain a rough approximation of the actual molecular geometry that could exist in free space. The resulting domain is as follows: Figure 4 Rotate as indicated by the black arrow in the diagram to facilitate visualization from different perspectives. For orientation, a segment of its edge is highlighted in blue.

[0272] from Figure 4 From a vertical perspective, ring disorder can be observed. The domain incorporates randomized splicing of 5-, 6-, and 7-membered rings. From a diagonal perspective, regions with positive curvature (indicated by red arrows) or negative curvature (orange arrows) can be observed. From a horizontal perspective, we can trace blue edge fragments, which provides a sense of z-direction lattice deflection (i.e., "z-deflection") caused by ring disorder. The z-deflection of the domain gives the edges a wavy shape, with the edges deflecting along the local lattice. As ring disorder increases, the amplitude and frequency of the edge z-deflection can increase.

[0273] V. Clarify the example

[0274] Analysis of the exemplary system provides a useful clarification of these concepts. Unless otherwise stated, the models depict sp 2 Hybrid or sp 3 It is a hybrid carbon atom and does not exhibit hydrogen atoms.

[0275] Figure 6 A consists of 26 numbered carbon atoms and is labeled R. A R B R C ... R H A system of eight ring structures. Labeled as R A The ring structure consists of seven carbon atoms (i.e., atoms 1, 2, 3, 4, 19, 20, and 21) bonded together in a covalent chain to form a closed heptagon. Therefore, R... A It satisfies the definition of a ring. Figure 6 All other cyclic structures in the molecule of A also satisfy the definition of a ring and can be expressed as a set of their atomic members.

[0276] R A In Figure 6 The side marked as x in A is also composed of the pentagonal ring R. C Shared. Because R A and R C They share a common edge, so it's also true that they share at least two atomic members. Therefore, ring R A and R C It satisfies the definition of an adjacent cycle.

[0277] exist Figure 6 In the system in A, each atom belongs to a ring, and each ring is connected to every other ring through at least one path from an adjacent ring. For example, ring R... A Many paths through adjacent rings (e.g., R) A →R C →R E , or R A →R H →R G →RE Connect to ring R E Therefore, the system can be described as a ring-connected graphene structure.

[0278] Next, we will evaluate Figure 6 The atoms in graphene structure A are used to determine whether they are internal or peripheral atoms. A R B and R C Therefore, 19 satisfies the definition of an internal atom. Atoms 20 through 26 also satisfy this definition. Each internal atom... Figure 1 The coloring is gray.

[0279] Atom 1 belongs to ring R, which does not completely surround it. A and R B Therefore, 1 satisfies the definition of an edge atom. Atoms 2 through 18 also satisfy this definition. All edge atoms are... Figure 1 The middle element is colored blue. Starting from any given edge atom, we can trace the chain of nearest neighbors from that first atom such that any two nearest neighbors within the chain are edge atoms and also co-members of exactly one ring. By continuing this tracing to its end, we define an edge.

[0280] For example, starting with 1, we find that 2 is the nearest neighbor, the edge atom, and exactly one ring (R). A The common members (along with 1) of the chain. Tracing this from 2 to 18, a closed loop is formed through the bonds between the last atom 18 in the chain and its nearest neighbor and the first atom 1 in the chain. These atoms together represent the edge of the graphene structure.

[0281] exist Figure 6 Figure B shows a system with 41 carbon atoms and 12 ring structures. Instead of numbering all the atoms, we characterize them into groups based on their color coding (gray, blue, and dark blue). Of the 12 ring structures, 11 satisfy the definition of a ring; the ring structure surrounded by 12 blue atoms contains more than 9 atomic members and is therefore not a ring. All 11 rings are linked together, and there are no atoms that are not rings; therefore, the entire system comprises a graphene structure.

[0282] Next, analysis Figure 6 The graphene structure in B consists of atoms. Only three atoms belong to a ring, and the ring is surrounded on all four sides. These internal atoms... Figure 6B is colored gray. Since the remaining 38 atoms in the graphene structure are all rings and not completely surrounded by rings, they are all edge atoms. Starting from any given edge atom, we trace the nearest neighbor chain such that any two nearest neighbors in the chain are edge atoms and co-members of exactly one ring. This results in edge tracing. Following this tracing rule, we find that we cannot perform tracing that includes all 38 edge atoms in the graphene structure. Therefore, once an edge is traced, we select any edge atom that is not yet assigned to an edge and trace a new edge, continuing this process until all edge atoms are assigned to edges. For... Figure 6 The system in B follows this procedure, and we can trace exactly two edges. The edge atoms that make up the 12-membered edge are colored blue, and the edge atoms that make up the 26-membered edge are colored dark blue.

[0283] exist Figure 6 Figure C illustrates a system comprising 66 carbon atoms and 21 ring structures. Instead of numbering all the atoms, we characterize them into groups based on their color coding (gray, black, blue, and dark blue). All 21 ring structures are rings, but not all rings are connected to all other rings. Instead, there is a first group of 14 rings connecting to each other and a second group of 7 rings connecting to each other, but neither group is connected to the other.

[0284] therefore, Figure 6 The system in C includes a 42-membered ring-linked graphene structure and a separate 24-membered graphene structure. Because Figure 6 In system C, all 66 atoms are members of a certain graphene structure, so the entire system can be represented as a graphene system. Furthermore, because the system includes two different graphene structures, it represents an assembly. Since the primary cohesive force between the two members is provided by the covalent bonds connecting them, the assembly includes bonded assemblies.

[0285] exist Figure 6 D shows a diagram containing 38 carbon atoms (all sp). 3 A system of 44 hydrogen atoms and 17 ring structures (hybridized carbon atoms). Instead of numbering all the atoms, we characterize them as groups based on their color coding (gray, light gray, and blue). The hydrogen atoms are all colored light gray and appear smaller than the carbon atoms. Each of the 17 ring structures consists of a 5-membered ring, and all 38 carbon atoms are members of one of the 17 rings. Each 5-membered ring is connected to every other 5-membered ring via path loops between adjacent rings, thus forming a ring-connected graphene structure.

[0286] because Figure 6The system in D includes atoms that are not ring members, and the graphene structure comprises polyatomic rings of carbon atoms; therefore, the system as a whole does not contain a graphene structure. However, the system does contain a graphene structure. Because most graphene structures will be bonded to hydrogen, oxygen, or other atoms, most graphene structures will be subsystems of a larger system that includes non-graphene structure elements. However, in this disclosure, we primarily limit our considerations to the polycyclic carbon arrangements that define the graphene structure.

[0287] exist Figure 6 In D, the graphene structure contains 15 carbon atoms that are both part of a ring and surrounded by rings on all four sides. These internal atoms are colored gray. The remaining 23 atoms in the graphene structure are part of a ring but not completely surrounded by rings. These edge atoms and the 23-membered edge they form are colored blue.

[0288] exist Figure 6 Figure E illustrates a graphene system. The graphene system comprises three distinct z-adjacent graphene members. Each graphene member is ring-broken relative to the other two graphene members, but is cohesive through interlayer vdW interactions. Therefore, Figure 6 The graphene system in E represents the vdW assembly.

[0289] exist Figure 7 Figure A shows a system comprising 42 carbon atoms and 15 ring structures. Figure 7 B and Figure 7 C indicates the isolated portion of this same system. The 15 ring structures in the system include 13 six-membered rings (labeled R1, R2, R...). 3个 ... R 13 All carbon atoms in the system are members of a ring, and all rings are path-connected to each other through at least one adjacent ring. Therefore, the entire 42-atom system comprises a single-ring connected graphene structure. This graphene monomer includes Y-dislocations, with cubic diamond-like seams at the intersections of these Y-dislocations. Figure 7 D is highlighted in yellow.

[0290] VI. Notes on Metrology and Characterization

[0291] A variety of different instruments were used to characterize the materials synthesized in this disclosure. The following discussion provides information about these instruments and the context of how we analyzed the relevant data.

[0292] All Raman spectral characterizations were performed using a ThermoFisher DXR Raman microscope equipped with a 532 nm excitation laser and Omnic line fitting software. Specific laser powers were used and specified where appropriate.

[0293] Raman spectroscopy is commonly used to characterize the molecular structure of carbon, and there is a wealth of literature on the subject. Two main spectral features are typically associated with sp. 2 Optical excitation of hybrid carbon is associated with: G-band (in graphite sp) 2 In carbon, typically at around 1580 cm⁻¹ -1 Up to 1585cm -1 (Exhibiting peak intensity values ​​at 1350 cm⁻¹) and D-band (at approximately 1350 cm⁻¹ under optical excitation). -1 (The peak intensity value is shown at this location). A second-order "2D" band, representing the D band, has also been observed in some graphitic carbons, and its peak intensity value is typically located at approximately 2700 cm⁻¹. -1 The G band belongs to sp. 2 -sp 2 The vibration of the bond. The D-band belongs to the sp-band arranged in the ring. 2 The radial breathing pattern of hybrid carbon atoms, and for Raman observation, this requires backscattering of electrons at defect sites.

[0294] Researchers have described the amorphization trajectory in the graphitic carbon spectrum, revealing the disorder progression from graphite to amorphous carbon, which helps in understanding the dynamics of the D band. In graphite, there is no D peak due to the absence of activation defects. In carbon including smaller graphene domains, the density of edge states increases, and with this increase in edge states, the D peak is activated by backscattering at edge defects. The D peak intensity increases toward the maximum value corresponding to nanocrystalline graphite. Further amorphization of the cyclic disordered form reduces the intensity of the D peak. Finally, further amorphization completely eliminates polycyclic sp... 2 Hybrid structure, D peak disappears.

[0295] with sp 3 The Raman spectral peaks associated with hybrid carbon include 1306 cm⁻¹. -1 The peak (associated with hexagonal diamond), 1325cm -1 The peak (associated with hexagonal diamond) and 1332cm -1 The peak at that point (associated with cubic diamond). Cubic diamond comprises 100% chair conformation, while hexagonal diamond comprises both chair and boat conformations, resulting in lower Raman frequencies and lower thermodynamic stability.

[0296] Raman-active phonons are known to be strain-dependent. Because the presence of strain within the lattice causes a shift in the vibrational frequencies of the lattice, Raman spectroscopy can be used to understand the strain state within the lattice. However, strain can also shift spectral peaks from their usual positions to new locations, making the identification more ambiguous. The main indicators of strain in cyclic disordered graphene structures are the positions of the G peak and the 2D peak, both of which are sensitive to tension and compression. The G peak has been shown to be located at sp... 2 -sp2 When bonds are stretched, they shift to lower frequencies (i.e., "redshift"), and when these bonds are compressed, they shift to higher frequencies (i.e., "blueshift"). Multiple modes of the G-band can exist in graphene structures with non-uniform strain fields.

[0297] In disordered carbon, several Raman spectral features were observed in addition to the D peak. These are typically observed in amorphous sp... 2 Hybridized carbon typically fits within 1500 cm⁻¹ -1 With 1550cm -1 The broad Raman peaks (sometimes referred to as D”) between the rings increase with ring disorder. This is attributed in this paper to the weakening of the sp-axis due to stretching. 2 -sp 2 The weakly correlated redshift pattern of the G-band associated with the bond, the pattern with sp 2 The G peak surges due to increased ring disorder and lattice distortion in the structure of hybrid graphene. Ferrari and Robertson have demonstrated that the G peak redshifts into this range in stage II of the amorphous trajectory. In graphene oxide, this redshift mode of the G peak can exist next to the normal G peak, thus indicating an intrinsic normal spt within the lattice. 2 There is a weak sp next to the key 2 This is consistent with the conventional interpretation of graphene oxide as a non-uniform lattice with both cyclic disorder and cyclic order regions.

[0298] Another feature observed in disordered carbon (called the D' peak) fits at 1620 cm⁻¹. -1 At this point, it can appear as a shoulder on the G peak. This feature is typically observed in sp[s] with high edge state density. 2 The hybrid carbon is accompanied by a D peak, and its intensity relative to the D peak has been shown to increase near the lattice edge.

[0299] Another feature observed in disordered carbon (sometimes called D) * The peak is fitted at 1100 cm⁻¹ -1 With 1200cm -1 The bandwidth between [the specified range]. 1175cm within this range. -1 The peak intensity value at that point is attributed to the presence of sp in the soot. 2 Network and SP 3 SP at the transition between networks 2 Atoms and sp 3 sp formed between atoms 2 -sp 3 The bond. It is also attributed to hexagonal diamond. Ferrari and Robertson, along with some researchers, attributed this peak to sp in nanodiamond and diamond-like materials. 3The carbon content is questionable, and the two individuals provided evidence suggesting that the peak should include -1240 cm⁻¹. -1 The broad peak at that point is attributed to trans-polyacetylene, i.e., protonated aliphatic sps demonstrably present in these carbons. 2 chain.

[0300] In this disclosure, Raman spectral analysis may involve references to unfitted or fitted spectral features. An “unfitted” spectral feature relates to spectral features that are apparent before deconvolution by linear fitting software. Therefore, an unfitted feature may represent the convolution of multiple underlying features, but their positions are not subjective. A “fitted” spectral feature relates to spectral features assigned by linear fitting software. Incomplete linear fitting indicates the possible presence of other underlying features that have not yet been deconvolved.

[0301] For clarity, features related to unfitted Raman curves are marked with the subscript "u"—for example, "G". u "Band. In this disclosure, OMNIC Peak Resolve software is used to perform linear fitting to deconvolve the features that contribute to the overall spectral line shape. These fitted features are labeled with "f"—for example, "D f "Band. The default Gaussian-Lorentz spectral shape setting uses the software, allowing the fitted band to employ both Gaussian and Lorentz characteristics, with fractional Gaussian characteristics determined by the software to optimize the fit. Other line shape fitting methods can change the position, intensity, and trend of the fitted peaks."

[0302] Another unfitted feature defined in this disclosure is the valley (“Tr”), which is the D in the overall spectral line shape. u With G u Regions with lower Raman intensity values ​​between bands. Tr u Strength is defined as D u Peak and G u The minimum intensity value that appears between peaks. Valley intensity values ​​indicate fundamental spectral dynamics, such as the redshift of the G band corresponding to ring disorder and lattice distortion, and can be analyzed without resorting to subjective line-fit judgments, thus making them practical features.

[0303] In this paper, the average Raman spectrum represents the average of multi-point spectral measurements of a sample obtained within a rectangular grid. The spectra at different points are normalized and then averaged to produce a composite spectrum.

[0304] X-ray diffraction of the toner was performed by the EAG laboratory. XRD data were collected by coupled θ:2θ scanning on a Rigaku Ultima-III diffractometer equipped with a copper X-ray tube with a Niβ filter, secondary focusing optics, a computer-controlled slit, and a D / teX Ultra 1D strip detector. Peak positions and widths were determined using line fitting software.

[0305] Thermogravimetric (TGA) analysis of the toner was performed on a TA Instruments Q600 TGA / DSC. Thermal oxidation studies were performed by heating the powder samples in air.

[0306] Transmission electron microscopy (TEM) imaging was performed on a FEI Tecnai F20 operating at 200 kV. A 300-mesh copper grid with lace carbon was used. All samples were prepared in ethanol and dried at room temperature.

[0307] Gas adsorption data can be collected using the Micromeritics Tristar II Plus at 77 K. The pressure is between and within a range Until Incremental nitrogen adsorption was measured. The BET specific surface area can be calculated using Micromeritics MicroActive software, assuming a cross-sectional area of ​​0.162 nm. 2 The data were derived from the BET monolayer capacity. All samples were pretreated by degassing with a continuous flow of dry nitrogen at 100°C prior to analysis, except for samples F2 and F3, which were degassed at 200°C prior to analysis.

[0308] Pore ​​size distribution (PSD) and pore volume accumulation are another technique that can be performed based on gas adsorption data to gain deeper insights into the sintering behavior of particles. Data were collected by Micromeritics Tristar II Plus at 77 K. The pressure is between and within a range Until Incremental measurements were performed on nitrogen adsorption and desorption. Samples were pretreated by degassing with a continuous flow of dry nitrogen at 100°C prior to analysis.

[0309] Micromeritics MicroActive software can be used to calculate adsorption-desorption PSD and pore volume accumulation by applying the Barrett, Joyner, and Halenda (BJH) method. This method provides a comparative evaluation of the mesopore size distribution in gas adsorption data. Faas correction and Harkins and Jura thickness curves can be applied to all BJH data. Pore volume accumulation can be measured for both the adsorption and desorption portions of the isotherm.

[0310] VII. Procedure

[0311] The following discussion outlines the procedures used to complete each study (i.e., studies A through G). We typically strive to label samples based on the study most relevant to them—that is, sample A1 is the first sample associated with study A. Within a single experiment, multiple samples may be evaluated, and multiple procedures may have been performed to create the samples. The procedures and sample labeling are identical—for example, “sample B2” was created using “procedure B2”.

[0312] This disclosure employs exemplary procedures. Other procedures (including those using pyrolysis with alternative solid or liquid carbonaceous precursor materials, alternative substrates or catalysts, or other basic parameters) may be used as alternatives to those described herein without departing from the concept of the invention. Several exemplary x-carbon synthesis procedures have been performed to establish the versatility of the methods, the synthetic mechanics, and certain observable trends that may be utilized.

[0313] Program—Research A

[0314] For programs A1, A2, and A3, a rotary tube furnace with a quartz tube can be used. The quartz tube can be a 60mm OD quartz tube containing a 12-inch middle section (“belly”) of a 100mm OD tube positioned within the heating zone of the furnace, such as... Figure 8 As shown in Figure A. The quartz baffle inside the furnace promotes powder agitation. The furnace can be kept horizontal (i.e., not tilted). Ceramic blocks can be inserted on each side of the furnace's heating zone (so that the powder sample is placed between the blocks and inside the heating zone). Glass wool can be used to hold the ceramic blocks in place. The powder sample can be placed into the tube without using a ceramic boat. The tube can be fitted with two stainless steel flanges. Gas can flow in through a gas inlet on one flange and out through a gas outlet in the other flange.

[0315] For procedures A4 and A5, a tube furnace with a quartz tube can be used. The quartz tube can be a 60mm OD tube. The furnace can be kept horizontal (i.e., not tilted). Ceramic blocks can be inserted on each side of the furnace's heating zone (so that the powder sample is placed between the blocks and inside the heating zone). The powder sample can be placed in an open ceramic boat inside the tube. The tube can be fitted with two stainless steel flanges. Gas can flow in through a gas inlet on one flange and out through a gas outlet in the other flange.

[0316] Using the furnace configuration described above, five carbon samples can be synthesized using the following procedure:

[0317] Procedure A1: A 500g sample of the magnesium oxide template precursor powder "Elastomag 170" (commercial magnesium oxide powder supplied by Akrochem) can be loaded into a quartz tube inside the heating zone of a tube furnace. The rotary tube furnace can be set to non-rotation mode. The furnace can be heated from room temperature to a set temperature of 1,050°C over 50 minutes with argon (Ar) gas at a flow rate of 500 sccm. The furnace can then be cooled to 750°C over the next 30 minutes under a continuous Ar flow. During this period, the MgO template precursor morphology can be altered to the desired template morphology due to calcination. This condition can be maintained for an additional 30 minutes, after which propylene (C3H6) gas can be initiated at a flow rate of 250 sccm while maintaining the Ar flow, and this condition can be maintained for 60 minutes. The C3H6 flow can then be interrupted, and the furnace cooled to room temperature under a continuous Ar flow. At this point, the synthesized C@MgO coated composite powder can be analyzed by Raman spectroscopy or thermogravimetric analysis (TGA). The MgO template can then be selectively extracted from the C@MgO-coated composite powder by acid etching with hydrochloric acid (HCl) under magnetic stirring, resulting in a mixture of carbon in an aqueous MgCl2 solution. The carbon is then filtered from the solution, washed three times with deionized water, and dried to form carbon powder. The carbon powder produced by this procedure is referred to herein as "Sample A1".

[0318] Procedure A2: A 500g sample of Elastomag 170 (commercial magnesium oxide powder supplied by Akrochem) magnesium oxide (MgO) template precursor powder is loaded into a quartz tube inside the heating zone of a tube furnace. The rotary tube furnace can be set to non-rotation mode. The furnace can be heated from room temperature to a set temperature of 1,050°C over 50 minutes with Ar gas at a flow rate of 500 sccm, and then maintained at this condition for 30 minutes. During this period, the MgO template precursor morphology can be changed to the desired template morphology due to calcination. Next, methane (CH4) gas can be initiated at a flow rate of 500 sccm while maintaining the Ar flow, and this condition can be maintained for 30 minutes. The CH4 flow can then be interrupted, and the furnace can be cooled to room temperature with a continuous Ar flow. At this point in the procedure, the synthesized C@MgO coated composite powder can be analyzed by Raman spectroscopy or thermogravimetric analysis (TGA). The MgO template can then be selectively extracted from the C@MgO-coated composite powder by acid etching with HCl under magnetic stirring, resulting in a mixture of carbon in an aqueous MgCl2 solution. The carbon is then filtered from the solution, washed three times with deionized water, and dried to form carbon powder. The carbon powder produced by this procedure is referred to herein as "Sample A2".

[0319] Procedure A3: MgO powder can be generated by calcining light magnesium carbonate (commercial magnesite powder supplied by Akrochem) at 1,050°C for 2 hours. A 300g sample of the pre-calcined powder can be loaded into a quartz tube inside the heating zone of a tube furnace. The rotary tube furnace can be set to rotate at 2.5 RPM. The furnace can be heated from room temperature to the set temperature of 650°C within 30 minutes with Ar gas at a flow rate of 500 sccm, and then maintained at this condition for 30 minutes. Next, a C3H6 gas flow of 270 sccm can be initiated while maintaining the Ar flow, and this condition can be maintained for 60 minutes. The C3H6 flow can then be interrupted and the furnace cooled to room temperature under a continuous Ar flow. At this point in the procedure, the synthesized C@MgO coated composite powder can be analyzed by Raman spectroscopy or thermogravimetric analysis (TGA). The MgO template can then be selectively extracted from the C@MgO-coated composite powder by acid etching with HCl under magnetic stirring, resulting in a mixture of carbon in an aqueous MgCl2 solution. The carbon is then filtered from the solution, washed three times with deionized water, and dried to form carbon powder. The carbon powder produced by this procedure is referred to herein as "Sample A3".

[0320] Program—Research B

[0321] For procedures B1-B3, MgO powder can be generated by calcining a template precursor powder containing rhombic magnesite (MgCO3) crystals. The precursor powder can be calcined in a Vulcan 3-550 muffle furnace at 580°C for 1 hour, followed by calcination at 1,050°C for 3 hours, with a heating ramp rate of 5°C / min.

[0322] For procedure B4, MgO powder can be generated by calcining a template precursor powder containing light magnesium carbonate crystals. The precursor powder can be calcined in a Vulcan 3-550 muffle furnace at 750°C for one hour, with a heating ramp rate of 5°C / min.

[0323] For programs B1-B3, an MTI rotary tube furnace and quartz tube can be used. The quartz tube can be a 60mm OD quartz tube containing a 12-inch middle section (“belly”) of a 100mm OD tube positioned within the heating zone of the furnace, such as... Figure 8 As shown in Figure A. The quartz baffle inside the furnace promotes powder agitation. The furnace can be kept horizontal (i.e., not tilted). Ceramic blocks can be inserted on each side of the furnace's heating zone (so that the powder sample is placed between the blocks and inside the heating zone). Glass wool can be used to hold the ceramic blocks in place. The powder sample can be placed into the tube without using a ceramic boat. The tube can be fitted with two stainless steel flanges. Gas can flow in through a gas inlet on one flange and out through a gas outlet in the other flange.

[0324] For procedure B4, a tube furnace with a quartz tube can be used. The quartz tube can be a 60mm OD tube. The furnace can be kept horizontal (i.e., not tilted). Ceramic blocks can be inserted on each side of the furnace's heating zone (so that the powder sample is placed between the blocks and inside the heating zone). The powder sample can be placed in an open ceramic boat inside the tube. The tube can be fitted with two stainless steel flanges. Gas can flow in through a gas inlet on one flange and out through a gas outlet in the other flange.

[0325] Procedure B1: A CVD procedure can be performed for 16 hours at 640°C under flowing gas conditions. The flowing gas may include 1,220 sccm of CO2 and 127 sccm of C3H6. The quartz tube can be rotated at 1 rpm. After the resulting C@MgO powder is cooled to room temperature under flowing CO2, the MgO template can be selectively extracted from the C@MgO-coated composite powder by acid etching with HCl under magnetic stirring, thereby producing a mixture of carbon in an aqueous MgCl2 solution. The carbon can then be filtered from the solution, washed three times with deionized water, and dried to form carbon powder. The carbon powder produced by this procedure is referred to herein as “Sample B1”.

[0326] Procedure B2: A CVD procedure can be performed for 20 hours at 580°C under flowing gas conditions. The flowing gas may include 1,220 sccm of CO2 and 127 sccm of C3H6. The quartz tube can be rotated at 1 rpm. After the resulting C@MgO powder is cooled to room temperature under flowing CO2, the MgO template can be selectively extracted from the C@MgO-coated composite powder by acid etching with HCl under magnetic stirring, thereby producing a mixture of carbon in an aqueous MgCl2 solution. The carbon can then be filtered from the solution, washed three times with deionized water, and dried to form carbon powder. The carbon powder produced by this procedure is referred to herein as "Sample B2".

[0327] Procedure B3: A CVD procedure can be performed for 32.5 hours at 540°C under flowing gas conditions. The flowing gas may include 1,220 sccm of CO2 and 127 sccm of C3H6. The quartz tube can be rotated at 1 rpm. After the resulting C@MgO powder is cooled to room temperature under flowing CO2, the MgO template can be selectively extracted from the C@MgO-coated composite powder by acid etching with HCl under magnetic stirring, thereby producing a mixture of carbon in an aqueous MgCl2 solution. The carbon can then be filtered from the solution, washed three times with deionized water, and dried to form carbon powder. The carbon powder produced by this procedure is referred to herein as “Sample B3”.

[0328] Procedure B4: A CVD procedure can be performed for 1 hour at 580°C under flowing gas conditions. The flowing gas may include 1,138 sccm of CO2 and 276 sccm of C2H2. After the resulting C@MgO powder is cooled to room temperature under flowing CO2, the MgO template can be selectively extracted from the C@MgO-coated composite powder by acid etching with HCl under magnetic stirring, thereby producing a mixture of carbon in an aqueous MgCl2 solution. The carbon can then be filtered from the solution, washed three times with deionized water, and dried to form carbon powder. The carbon powder produced by this procedure is referred to herein as "Sample B4".

[0329] Program—Research C

[0330] For procedures C1 and C2, MgO powder can be generated by processing template precursor powder containing elongated sodium-doped magnesite template precursor crystals. The sodium-doped magnesite template precursor can be precipitated from a stock solution of magnesium bicarbonate. First, a 0.62 mol / kg solution of magnesium hydroxide (Akrochem Versamag) and deionized water can be prepared in a 57-liter pressure vessel. -1 A mixture of Mg. This mixture can be recycled by carbonization with up to 60 psig of CO2 to form a stock solution of magnesium bicarbonate (Mg(HCO3)2). After approximately 22 hours, the solution can be filtered to remove undissolved solids. The resulting stock solution has a concentration of 0.29 mol / kg. -1 Mg. Then, sodium bicarbonate (NaHCO3) can be added to the stock solution to bring the sodium concentration in the system to 1.7 × 10⁻⁶. -3 mol kg -1 Na. Additional CO2 can be added to the container for 20 minutes to digest any unwanted precipitates. The system can be heated to 34°C and depressurized to allow crystallization over 25.5 hours. The mixture formed by crystallization of the sodium-doped elongated trihydrate magnesite template precursor crystals can then be filtered, washed with deionized water and acetone, and dried at 45°C in a forced air recirculation oven. The template precursor can be used as is in the CVD replication step, and the conversion to MgO occurs in situ during the heated ramp stage.

[0331] For procedures C1 and C2, a tube furnace with a quartz tube can be used. The quartz tube can be a 60mm OD tube. The furnace can be kept horizontal (i.e., not tilted). Ceramic blocks can be inserted on each side of the furnace's heating zone (so that the powder sample is placed between the blocks and inside the heating zone). The powder sample can be placed in an open ceramic boat inside the tube. The tube can be fitted with two stainless steel flanges. Gas can flow in through a gas inlet on one flange and out through a gas outlet in the other flange.

[0332] Program C1:

[0333] A 1.6g sample of a sodium-doped, elongated magnesite template precursor can be loaded into a quartz tube inside the heating zone of a tube furnace. The furnace can be heated from room temperature to a set temperature of 460°C within 20 minutes under Ar gas at a flow rate of 1271 sccm, and then held at this condition for 15 minutes to equilibrate. Next, a C2H2 gas flow of 42 sccm can be initiated while maintaining a constant Ar flow, and this condition can be maintained for 3 hours. The C2H2 flow can then be interrupted, and the furnace cooled to room temperature under a continuous Ar flow, allowing the resulting C@MgO powder to be collected. The MgO template can be selectively extracted from the C@MgO-coated composite powder by acid etching with HCl under magnetic stirring, resulting in a mixture of carbon in an aqueous MgCl2 solution. The carbon can then be filtered from the solution, washed three times with deionized water, and dried to form carbon powder. The carbon powder produced by this procedure is referred to herein as “Sample C1”.

[0334] Program C2

[0335] A 1.9g sample of a sodium-doped, elongated magnesite template precursor can be loaded into a quartz tube inside the heating zone of a tube furnace. The furnace can be heated from room temperature to a set temperature of 400°C within 20 minutes under Ar gas at a flow rate of 1271 sccm, and then held at this condition for 15 minutes to equilibrate. Next, a C2H2 gas flow of 105 sccm can be initiated while maintaining the Ar flow, and this condition can be maintained for 3 hours. The C2H2 flow can then be interrupted, and the furnace cooled to room temperature under a continuous Ar flow, allowing the resulting C@MgO powder to be collected. The MgO template can be selectively extracted from the C@MgO-coated composite powder by acid etching with HCl under magnetic stirring, resulting in a mixture of carbon in an aqueous MgCl2 solution. The carbon can then be filtered from the solution, washed three times with deionized water, and dried to form carbon powder. The carbon powder produced by this procedure is referred to herein as “Sample C2”.

[0336] Program—Research D

[0337] For procedures D1 and D2, MgO powder can be generated by calcining a template precursor powder containing light magnesium carbonate crystals. The precursor powder can be calcined in a Vulcan 3-550 muffle furnace at 750°C for one hour, with a heating ramp rate of 5°C / min.

[0338] For procedures D1 and D2, a tube furnace with a quartz tube can be used. The quartz tube can be a 60mm OD tube. The furnace can be kept horizontal (i.e., not tilted). Ceramic blocks can be inserted on each side of the furnace's heating zone (so that the powder sample is placed between the blocks and inside the heating zone). The powder sample can be placed in an open ceramic boat inside the tube. The tube can be fitted with two stainless steel flanges. Gas can flow in through a gas inlet on one flange and out through a gas outlet in the other flange.

[0339] Program D1

[0340] A 0.9 g sample of the magnesium oxide template precursor can be loaded into a quartz tube inside the heating zone of a tube furnace. The furnace can be heated from room temperature to a set temperature of 700 °C within 30 minutes under Ar gas at a flow rate of 1271 sccm, and then held at this condition for 15 minutes to equilibrate. Next, a C3H6 gas flow of 20 sccm can be initiated while maintaining a constant Ar flow, and this condition can be maintained for 30 minutes. The C3H6 flow can then be interrupted, and the furnace can be cooled to room temperature under a continuous Ar flow, allowing the resulting C@MgO powder to be collected. The MgO template can be selectively extracted from the C@MgO-coated composite powder by acid etching with HCl under magnetic stirring, resulting in a mixture of carbon in an aqueous MgCl2 solution. The carbon can then be filtered from the solution, washed three times with deionized water, and dried to form carbon powder. The carbon powder produced by this procedure is referred to herein as “Sample D1”.

[0341] Program D2

[0342] A 0.9 g sample of the magnesium oxide template precursor can be loaded into a quartz tube inside the heating zone of a tube furnace. The furnace can be heated from room temperature to a set temperature of 700 °C within 30 minutes under an argon (Ar) flow rate of 1271 sccm, and then held at this condition for 15 minutes to equilibrate. Next, a combination of propylene (C3H6) gas at a flow rate of 20 sccm and hydrogen (H2) gas at a flow rate of 60 sccm can be initiated while maintaining the Ar flow constant, and this condition can be maintained for 30 minutes. The C3H6 flow is then interrupted, and the furnace is cooled to 150 °C under continuous Ar and H2 flow. The H2 flow can be interrupted below 150 °C, and the furnace cooled to room temperature, allowing the resulting C@MgO powder to be collected. The MgO template can be selectively extracted from the C@MgO-coated composite powder by acid etching with HCl under magnetic stirring, resulting in a mixture of carbon in an aqueous MgCl2 solution. The carbon can then be filtered from the solution, washed three times with deionized water, and dried to form carbon powder. The carbon powder produced by this process is referred to in this paper as “Sample D2”.

[0343] Program—Research E

[0344] For procedures E1 and E2, MgO powder can be produced by calcining light magnesium carbonate (commercial magnesite powder supplied by Akrochem) in a rotary kiln in an air atmosphere in two stages, as shown below. Figure 8 As shown in A, the first stage of heat treatment can be performed at 400°C with a powder residence time of 9 minutes, followed by a second stage of heat treatment at 750°C with a powder residence time of 3 minutes.

[0345] For programs E1A and E2A, a tube furnace with a quartz tube can be used. For CVD, an MTI rotary tube furnace with a 60mm OD quartz tube can be used. The furnace can be kept horizontal (i.e., not tilted). Ceramic blocks can be inserted on each side of the furnace's heating zone (so that the powder sample is placed between the blocks and inside the heating zone). Glass wool can be used to fix the position of the ceramic blocks. The tube can be fitted with two stainless steel flanges. Gas can flow in through a gas inlet on one flange and out through a gas outlet in the other flange. The powder sample can be placed in a ceramic boat, and the boat can be placed in the heating zone before initiating the program. For programs E2 and E4, a similar setup can be used, with only minor modifications for rapid heating and / or cooling of the sample. These modifications will be described in their respective exemplary programs.

[0346] Procedure E1: A 50mm OD quartz tube containing 62g of this pre-calcined MgO powder, used as a boat, can be loaded into the furnace. After initiating an Ar gas flow at a flow rate of 2,000 sccm, the furnace can be heated from room temperature to a set temperature of 700°C within 20 minutes and maintained at this temperature for 15 minutes. Next, a C3H6 gas flow rate of 1,274 sccm can be initiated while maintaining the Ar flow, and this condition can be maintained for 30 minutes. The C3H6 flow can then be interrupted, and the furnace can be cooled to room temperature under a continuous Ar flow. The C@MgO coated composite powder can then be collected.

[0347] The MgO template can be selectively extracted from the C@MgO coated composite powder by acid etching with HCl under magnetic stirring, resulting in a mixture of carbon in an aqueous MgCl2 solution. The carbon can then be filtered from the solution, washed three times with deionized water, and dried to form carbon powder. The carbon powder produced by this procedure is referred to herein as "Sample E1".

[0348] Procedure E1A: This procedure involves rapidly heating and cooling the coated composite material from room temperature to a desired temperature setting. 3.0 g of the coated composite powder described in Procedure E1 is loaded into a ceramic boat and placed in a quartz tube outside the heating zone of the furnace. After initiating an Ar gas flow rate of 4,000 sccm, the furnace can be heated from room temperature to the temperature setting of 900°C within 45 minutes and held at this condition for 15 minutes. The sample can be held outside the heating zone until the temperature setting has been reached. Once the desired temperature has been reached, the boat is pushed into the heating zone with minimal additional air introduction and held there for 30 minutes, after which it is moved back into the quartz tube outside the heating zone. This can be used to expose the sample to the desired temperature for only a short period. The furnace can be cooled to room temperature under a continuous Ar flow. The C@MgO coated composite powder can be collected at room temperature.

[0349] The MgO template can be selectively extracted from the C@MgO coated composite powder by acid etching with HCl under magnetic stirring, resulting in a mixture of carbon in an aqueous MgCl2 solution. The carbon can then be filtered from the solution, washed three times with deionized water, and dried to form carbon powder. The carbon powder produced by this procedure is referred to herein as "Sample E1A".

[0350] Procedure E2: A 50 mm OD quartz tube containing 74 g of this pre-calcined MgO powder, used as a boat, can be loaded into the furnace. After initiating an Ar gas flow at a rate of 2,000 sccm, the furnace can be heated from room temperature to a set temperature of 580°C within 20 minutes and maintained at this temperature for 15 minutes. Next, a C3H6 gas flow at a rate of 1,274 sccm can be initiated while maintaining the Ar flow, and this condition can be maintained for 3 hours. The C3H6 flow can then be interrupted, and the furnace can be cooled to room temperature under a continuous Ar flow. The C@MgO coated composite powder can then be collected.

[0351] The MgO template can be selectively extracted from the C@MgO coated composite powder by acid etching with HCl under magnetic stirring, resulting in a mixture of carbon in an aqueous MgCl2 solution. The carbon can then be filtered from the solution, washed three times with deionized water, and dried to form carbon powder. The carbon powder produced by this procedure is referred to herein as "Sample E2".

[0352] Procedure E2A: This procedure involves gradually heating the coated composite material from room temperature to a desired temperature setting and then rapidly cooling it back to room temperature. 3.0 g of the coated composite powder described in Procedure E3 can be loaded into a ceramic boat and placed in a quartz tube within the heated zone of the furnace. After initiating an Ar gas flow of 4,000 sccm, the furnace can be heated from room temperature to the set temperature of 1,050°C over 50 minutes and held at this temperature for 15 minutes. The furnace can be held at this temperature for one hour. The furnace can then be allowed to begin cooling under a continuous Ar flow, and the ceramic boat can be pulled out of the heated zone as soon as the heater is de-energized. Once at room temperature, the C@MgO coated composite powder column can be collected.

[0353] The MgO template can be selectively extracted from C@MgO-coated composite powder by acid etching with HCl under magnetic stirring, resulting in a mixture of carbon in an aqueous MgCl2 solution. The carbon can then be filtered from the solution, washed three times with deionized water, and dried to form carbon powder. The carbon powder produced by this procedure is referred to herein as "Sample E2A".

[0354] Program—Research F

[0355] For procedure F1, MgO powder can be generated by calcining a template precursor powder containing light magnesium carbonate crystals. The precursor powder can be calcined in a Vulcan 3-550 muffle furnace at 750°C for one hour, with a heating ramp rate of 5°C / min.

[0356] For program F1, a Thermcraft tube furnace modified into a rotary furnace with a quartz tube can be used. The quartz tube can be a 60mm OD quartz tube containing an extended 577mm section (“belly”) of a 130mm OD tube positioned within the heating zone of the furnace. Quartz baffles inside the belly facilitate powder agitation. The furnace can be kept horizontal (i.e., not tilted). The template sample can be placed inside the belly within the heating zone, with ceramic blocks inserted on the outside of the belly on each side of the heating zone of the furnace. Glass wool can be used to secure the ceramic blocks. The template sample can be placed in the tube without using a ceramic boat, allowing the template sample to rotate freely within the belly. The tube can be fitted with two stainless steel flanges. Gas can flow in through a gas inlet on one flange and out through a gas outlet in the other flange.

[0357] For programs F2, F3, F4, F5, F6, and F7, a tube furnace with a quartz tube can be used. For CVD, an MTI rotary tube furnace with a 60mm OD quartz tube can be used. The furnace can be kept horizontal (i.e., not tilted). Ceramic blocks can be inserted on each side of the furnace's heating zone (so that the powder sample is placed between the blocks and inside the heating zone). Glass wool can be used to fix the position of the ceramic blocks. The tube can be fitted with two stainless steel flanges. Gas can flow in through a gas inlet on one flange and flow out through a gas outlet in the other flange. The powder sample can be placed in a ceramic boat, and the boat can be placed in the heating zone before initiating the program.

[0358] Procedures F1 and F2: 150 g of magnesium oxide template powder is loaded into the belly of a quartz tube. After initiating a CO2 gas flow rate of 1,379 sccm and a tube rotation speed of 1 RPM, the furnace is heated from room temperature to a temperature setting of 580°C at an ramp rate of 20°C / min and held at this condition for 15 minutes. Next, a C2H2 gas flow rate of 276 sccm is initiated while maintaining the CO2 flow, and this condition is maintained for 180 minutes. The C2H2 flow is then interrupted, and the furnace is cooled to room temperature under a continuous CO2 flow. The powder is collected. The C@MgO coated composite powder can be further processed to produce carbon powder. The MgO template can be selectively extracted from the C@MgO coated composite powder by acid etching with HCl under magnetic stirring, resulting in a mixture of carbon in an aqueous MgCl2 solution. The carbon is then filtered from the solution, washed three times with deionized water, further washed three times with ethanol, and dried to obtain carbon powder, referred to herein as “Sample F1”.

[0359] A 50 mg sample of carbon powder (Sample F1) can be compacted in a 7 mm module (Pike Technologies 161-1010) under 105 ksi hydraulic pressure. Under pressure, the carbon forms flakes that are sufficiently stable for processing; these flakes are referred to herein as “Sample F2”.

[0360] Procedure F3: Sample F2 can be placed in a ceramic boat and inserted into the quartz tube of the furnace. After initiating an Ar gas flow rate of 4,000 sccm, the furnace can be heated from room temperature to a temperature setting of 1,050°C over 50 minutes and maintained at this condition for 30 minutes. The furnace can then be cooled to room temperature under a continuous Ar flow. Once at room temperature, the flakes can be collected, and these flakes are referred to herein as “sample F3”.

[0361] Procedure F4: Place 100 mg of sample F1 powder in a ceramic boat and load it into the quartz tube of the furnace. After initiating an Ar gas flow rate of 4,000 sccm, heat the furnace from room temperature to the set temperature of 1050°C over 50 minutes and maintain this temperature for 30 minutes. Then allow the furnace to cool to room temperature under a continuous Ar flow. Once at room temperature, the powder can be collected.

[0362] This powder, in an amount of 50 mg, can then be compacted in a 7 mm module (Pike Technologies 161-1010) under 105 ksi hydraulic pressure. Under pressure, the coated carbon framework does not form granules and remains a powder, which is referred to herein as sample F4.

[0363] Procedure F5: Potassium carbonate (K₂CO₃) template precursors can be spray-dried using a Sinoped LPG-5 spray dryer. A room temperature solution consisting of 250.35 g of K₂CO₃ and 1,667.2 g of deionized water (DI) is pumped into a rotary atomizer set to 24,000 RPM at a rate of 23 mL / min. The inlet temperature of the spray dryer is set to 195 °C, resulting in an outlet temperature of 139 °C. The powder collected after spray drying is the K₂CO₃ template precursor.

[0364] 100 g of this K2CO3 template precursor powder can be loaded into a ceramic boat and placed in a quartz tube to generate coated composite powder using an MTI tube furnace. After initiating a CO2 gas flow at 1,220 sccm, the furnace can be heated from room temperature to a temperature setting of 640°C at an incline rate of 20°C / min and held at this condition for 15 minutes. Next, a C3H6 gas flow at 162 sccm can be initiated while maintaining the CO2 flow, and this condition can be maintained for 2 minutes. The C3H6 flow can then be interrupted, and the furnace can be purged with Ar at a flow rate of 2,000 sccm for 30 minutes to remove all CO2 present in the tube. The furnace can then be cooled to room temperature under a continuous Ar flow. The powder can be collected. The C@K2CO3 coated composite powder can be further processed to produce carbon powder. The K2CO3 template can be selectively extracted from the C@K2CO3 coated composite powder by acid etching with HCl under magnetic stirring conditions, thereby producing a mixture of carbon in an aqueous KCl2 solution. The carbon can then be filtered out of the solution, and the mixture can be washed three times with deionized water to obtain an aqueous paste. This paste can then be washed three times with ethanol to obtain an ethanol paste.

[0365] The ethanol paste of this carbon can be diluted with additional ethanol to produce a very dilute 0.003 wt% carbon mixture. This mixture can then be agitated for 5 minutes using an IKA T-25 digital Ultra-Turrax (UT) high-shear rotor-stator homogenizer running at 12,000 RPM. The agitated mixture can be immediately poured onto a glass frit vacuum filter with a 47 mm diameter nylon filter (0.45 μm pore size) as the filter medium. Vacuum filtration can proceed undisturbed until all liquid has been drained. The vacuum is then shut off, and the carbon-containing filter can be dried in air within the vacuum filter itself. Once dried, the flexible vdW assembly can be released from the filter. This vdW assembly is referred to herein as “Sample F5”.

[0366] Procedure F6: Sample F5 can be placed in a ceramic boat and inserted into the quartz tube of the furnace. After initiating an Ar gas flow rate of 4,000 sccm, the furnace can be heated from room temperature to a temperature setting of 1,050°C over 50 minutes and maintained at this condition for 30 minutes. The furnace can then be cooled to room temperature under a continuous Ar flow. Once at room temperature, the assembly can be collected, and said assembly is referred to herein as "sample F6".

[0367] Procedure F7: Magnesium carbonate trihydrate (MgCO3·3H2O) can be precipitated from hydrated magnesite (MgCO3·5H2O) to produce elongated particles. A 45 g / L MgO equivalent magnesium bicarbonate (Mg(HCO3)2) solution can be prepared by high-pressure dissolution of magnesium hydroxide in carbonic acid at 720 psig (Akrochem Versamag). The hydrated magnesite can be precipitated from this magnesium bicarbonate solution in a continuously stirred reactor (CSTR). The solution can be cooled to approximately 14°C and depressurized from 720 psig to 0 psig over 5 minutes while agitating at approximately 700 RPM using a submersible impeller. Air can be introduced at 4 SCFM while cooling to approximately 12°C. 空气 The solution was continuously purged through the headspace for 8 hours. An additional 18.5 hours of stirring at -350 RPM was permitted. The CSTR was then heated to 34.5°C while stirring at -720 RPM for 82 minutes. The solution was then diluted with approximately 5 L of deionized water while continuing heating to 43.8°C for another 61 minutes. The contents of the CSTR were then removed, filtered, and dried in a forced-air circulating oven at 40°C. The resulting powder, designated as N2 herein, is needle-like crystals of magnesite trihydrate.

[0368] MgO powder can be generated by calcining N2 in a 2,000 sccm N2 stream at 640°C for 2 hours in an MTI tube furnace with a 60 mm diameter quartz tube at a heating ramp rate of 5°C / min. 2.4 g of this MgO powder can be loaded into a ceramic boat and placed in a quartz tube to generate C@MgO using an MTI tube furnace. After initiating a CO2 gas flow of 815 sccm, the furnace can be heated from room temperature to the set temperature of 540°C at a ramp rate of 5°C / min and held at this condition for 15 minutes. Next, a C2H2 gas flow of 812 sccm can be initiated while maintaining the CO2 flow, and this condition can be maintained for 2 minutes. The C2H2 flow can then be interrupted, and the furnace can be purged with Ar at a flow rate of 1,698 sccm for 30 minutes to remove all CO2 present in the tube. The furnace can then be heated to 900°C at a ramp rate of 20°C / min and held at this condition for 30 minutes. The furnace can then be cooled to room temperature under a continuous flow of Ar. The powder can be collected. The C@MgO coated composite powder can be further processed to produce carbon powder. The MgO template can be selectively extracted from the C@MgO coated composite powder by acid etching with HCl under magnetic stirring, thereby producing a mixture of carbon in an aqueous MgCl2 solution. The carbon can then be filtered out of the solution and washed three times with deionized water to obtain an aqueous paste. This paste can be washed three times with ethanol to obtain an ethanol paste.

[0369] The ethanol paste of this carbon can be diluted with additional ethanol to produce a very dilute 0.003 wt% carbon mixture. This mixture can then be agitated for 5 minutes using an IKA T-25 digital Ultra-Turrax (UT) high-shear rotor-stator homogenizer running at 12,000 RPM. The agitated mixture can be immediately poured onto a glass frit vacuum filter with a 47 mm diameter nylon filter (0.45 μm pore size) as the filter medium. Vacuum filtration can proceed undisturbed until all liquid has been drained. The vacuum is then shut off, and the carbon-containing filter can be dried in air within the vacuum filter itself. Once dried, the viscous flexible buck paper can be released from the filter, referred to herein as “sample F7”.

[0370] Program—Research G

[0371] Program G1: Magnesite (MgCO3) particles can be crystallized from magnesium bicarbonate solution to produce equiaxed template precursor particle powder.

[0372] An MTI rotary tube furnace and quartz tube can be used. The quartz tube can be a 60mm OD quartz tube, containing a 12-inch section of a 100mm OD tube positioned within the heating zone of the furnace, such as... Figure 8As shown in Figure A. The quartz baffles inside the furnace promote powder agitation. The furnace can be kept horizontal (i.e., not tilted). Ceramic blocks can be inserted on each side of the furnace's heating zone (so that the powder sample is placed between the blocks and inside the heating zone). Glass wool can be used to fix the position of the ceramic blocks. The tube can be fitted with two stainless steel flanges. Gas can flow in through a gas inlet on one flange and out through a gas outlet in the other flange.

[0373] 177g of precipitated magnesite powder was heated at 640°C for 5ft. 3 Calcination is performed for 10 min at an Ar gas flow rate of 20 °C / min to produce MgO. Pre-existing MgO powder in the quartz tube can be used to generate C@MgO using the furnace. After initiating a CO2 gas flow rate of 1,918 sccm and a tube rotation speed of 1 RPM, the furnace can be heated from room temperature to a temperature setting of 640 °C at an incline rate of 20 °C / min and held at this condition for 15 min. Next, a C3H6 gas flow rate of 127 sccm can be initiated while maintaining the CO2 flow, and this condition can be maintained for 360 min. The C3H6 flow can then be interrupted, and the furnace can be cooled to room temperature under a continuous CO2 flow.

[0374] The C@MgO coated composite powder can be placed in a tube within an identical furnace / tube configuration for a second growth cycle. After initiating a CO2 gas flow rate of 1,918 sccm and a tube rotation speed of 1 RPM, the furnace can be heated from room temperature to a temperature setting of 640°C at an ramp rate of 20°C / min and held at this condition for 15 minutes. Next, a C3H6 gas flow rate of 127 sccm can be initiated while maintaining the CO2 flow, and this condition can be maintained for 120 minutes. The C3H6 flow can then be interrupted, and the furnace can be cooled to room temperature under a continuous CO2 flow.

[0375] The C@MgO coated composite powder can be placed in a tube within an identical furnace / tube configuration for a third growth cycle. After initiating a CO2 gas flow rate of 1,918 sccm and a tube rotation speed of 1 RPM, the furnace can be heated from room temperature to a temperature setting of 640°C at an ramp rate of 20°C / min and held at this condition for 15 minutes. Next, a C3H6 gas flow rate of 127 sccm can be initiated while maintaining the CO2 flow, and this condition can be maintained for 180 minutes. The C3H6 flow can then be interrupted, and the furnace can be cooled to room temperature under a continuous CO2 flow.

[0376] The powder can be collected. The C@MgO-coated composite powder can be further processed to produce carbon powder. The MgO template can be selectively extracted from the C@MgO-coated composite powder by acid etching with HCl under magnetic stirring, resulting in a mixture of carbon in an aqueous MgCl2 solution. The carbon can then be filtered from the solution, washed three times with deionized water, and then washed three times with ethanol to obtain an ethanol paste. This paste can be dried to form carbon powder.

[0377] This carbon powder can then be used for further CVD growth. An MTI rotary tube furnace with a quartz tube can be used. The quartz tube can be a 60mm OD quartz tube containing a 12-inch section of a 100mm OD tube positioned within the furnace's heating zone. A quartz baffle inside the furnace promotes agitation of the carbon powder. The furnace can be kept horizontal (i.e., not tilted). Ceramic blocks can be inserted on each side of the furnace's heating zone (so that the powder sample is placed between the blocks and inside the heating zone). Glass wool can be used to secure the ceramic blocks. The tube can be fitted with two stainless steel flanges. Gas can flow in through a gas inlet on one flange and out through a gas outlet in the other flange. This assembly... Figure 8 As shown in A.

[0378] After initiating a CO2 gas flow rate of 1,918 sccm and a tube rotation speed of 1 RPM, the furnace can be heated from room temperature to a temperature setting of 640°C at an ramp rate of 20°C / min and held at this condition for 15 minutes. Next, a C3H6 gas flow rate of 127 sccm can be initiated while maintaining the CO2 flow, and this condition can be maintained for 180 minutes. The C3H6 flow can then be interrupted and the furnace cooled to room temperature under a continuous CO2 flow. The final mass of the collected carbon powder, after deducting losses due to migration into the glass wool, is approximately 43.2 g. The carbon powder produced by this procedure is referred to herein as “Sample G1”.

[0379] Program—Research H

[0380] Procedure H: An aqueous solution of Mg(HCO3)2 can be produced by mixing 16 kg of deionized water and 1.39 kg of commercial-grade MgO powder (Versamag) in a pressure vessel equipped with a top stirring system and a self-priming impeller. The mixture can be mixed at 700 RPM and cooled to 5°C while being fed with CO2 gas at up to 850 psi for 2 hours. The resulting solution can be extracted from the pressure vessel at atmospheric pressure and fed at a rate of 56 mL / min into a BETEXA air atomizing nozzle comprising an FC7 liquid cap and an AC1802 gas cap. Compressed air for droplet atomization can be delivered to the nozzle at a flow rate of 54 psi and 5 SCFH. The inlet temperature of the spray dryer can be set to 200°C, resulting in an outlet temperature ranging from 108°C to 109°C. Ambient conditions during the spray drying process can be 28.4°C and 48% RH. Approximately 1400 mL of solution can be sprayed, and 208 g of spray-dried hydrous magnesium carbonate (Mg(CO3)·xH2O) template precursor powder with a hollow spherical morphology can be collected by a cyclone separator.

[0381] Next, the template precursor powder can be converted into a template through heat treatment using a muffle furnace (Vulcan 3-550, maximum 1440W). Approximately 10g of template precursor powder can be placed in a ceramic boat and heated to 580°C, then held at this temperature for 13.5 hours, followed by heating to 1050°C and holding for an additional hour to produce approximately 3.9g of MgO powder. The heating ramp rate for both steps can be 5°C / min, and cooling can be allowed to occur naturally over an overnight period of 8 hours. Approximately 0.47g of MgO powder can be granulated in a 15.7mm ID hydraulic press by applying a uniaxial compression of 7.8ksi for 1 minute. The resulting disc-shaped template can have a diameter of 15.7mm and a thickness of 2.5mm.

[0382] Next, a template-guided CVD process can be performed using a Thermcraft tube furnace with a 60mm OD quartz tube. Before initiating the process, the furnace should be kept horizontal (i.e., not tilted), and a 0.47g granulation template sample should be placed in the heating zone in a ceramic boat. Ceramic blocks can be inserted externally on each side of the furnace's heating zone, and their position can be secured using glass wool. The tube can be fitted with two stainless steel flanges. Gas can flow in through a gas inlet on one flange and out through a gas outlet in the other flange. After initiating a CO2 gas flow at 815 sccm, the furnace can be heated from room temperature to a temperature setting of 540°C at an ramp rate of 20°C / min and held at this condition for 5 minutes. Next, a C2H2 gas flow at 144 sccm can be initiated while maintaining the CO2 flow, and this condition can be maintained for 90 minutes. The C2H2 flow can then be interrupted, and the furnace can be cooled to room temperature with a continuous CO2 flow. During cooling, the clamshell furnace lid can be fully opened, exposing the quartz tube to the outside air. The coated composite particles obtained after cooling can be characterized. Finally, the same CVD growth procedure can be repeated twice, with the particles cooled again, for a total of three CVD growth steps, with the particles cooled between each step. The resulting coated composite particles include macroscopic coated carbon that can be used to test environmental superconductivity.

[0383] Vacuum chambers associated with systems like the Cober-Muegge microwave system used in research G can be utilized. Figure 8 C) A vacuum chamber, but without any microwave radiation. The vacuum chamber can be equipped with a 4-point probe (Lucas / Signatone SP4-40045TFJ) for measuring leadless sheet resistance and contact resistance. Probe specifications can be a 40 mil pitch between tungsten carbide tips, a 5 mil tip radius, and a 45 g spring pressure. The 4-point probe can be placed inside the vacuum chamber and wired to a Keithley Series 2400 source meter located outside the vacuum chamber. The Keithley source meter can be set to 4-wire mode with the automatic ohmmeter method selected and operates as a conventional constant current source ohmmeter with a starting current of 10 mA. With the auto-ranging function selected, the current steps up to 100 mA if the measured resistance drops below 20 ohms / square. The chamber pressure can be measured in parallel with the sheet resistance of the sample using a convection-enhanced Pirani vacuum gauge module (CVM201 Super Bee), which is capable of readings down to 0.1 holothrix with a resolution accuracy of 0.1 holothrix and a reading repeatability of 2%. Finally, the chamber may be equipped with a vacuum pump. This setup should allow the vacuum chamber to be evacuated while simultaneously reading the chamber pressure and sheet resistance.

[0384] The tips of the four-point probes should be positioned as gently as possible to make static contact with the flat surface of the macrostructure to obtain stable, continuous sheet resistance readings. This careful positioning should be avoided to prevent the probe tips from compressing the macrostructure surface, as the sp... x The macroscopic body exhibits significant pressure sensitivity, which may be necessary. We hypothesize that this pressure sensitivity is attributable to localized mechanical compression reducing the interlayer distance and thereby inducing interlayer electronic coupling near the voltage-sensing contact point. Additionally, a soft, non-conductive backing can be used beneath the carbon macroscopic body to minimize localized compression. To establish contact, the source meter can be opened to obtain initial readings under ambient conditions, after which the chamber can be sealed and evacuated. During chamber evacuation, readings of chamber pressure and sample sheet resistance can be recorded.

[0385] VIII. Study A—Analysis

[0386] The SEM image of sample A1 confirms the presence of the encapsulated frame. Figure 9 This is a SEM micrograph of sample A1 after the content phase of the coated composite powder has been removed. It is unclear whether one or more different coated frameworks exist in this SEM micrograph. The morphology appears to consist of jointly formed macroporous subunits (in...). Figure 9 The composition (marked in the middle) reflects the template used for partially sintered powder. This is in contrast to the sample to be studied in sample A2, which appears fragmented and deformed after liquid-phase treatment and evaporative drying (as shown in the image). Figures 21 to 22 The framework shown is different. Figure 9 The framework in the sample appears to have remained largely intact and was essentially unaffected by the processing and drying. This suggests that the coated walls in sample A1 were better able to withstand the stresses encountered during processing.

[0387] To achieve better transparency and to investigate the smaller-scale structure of the envelope wall in sample A1, TEM analysis was also performed. Figure 10 A is a TEM micrograph where we can observe a typical framework against a lace carbon background grid (this grid is used to support the TEM sample and is not the carbon of interest). The framework in this micrograph appears to include... Figure 10 At least nine macroporous subunits, numbered A. The cavities matched the morphology of the removed contents (not imaged) in both size and shape. No signs of buckling or wrinkling were found within the walls.

[0388] exist Figure 10The higher magnification view shown in B allows for a closer examination of the coated walls. This image shows a cross-section of the walls. Some walls observed in sample A1 are consistently as thick as -12 nm (or -30 to -35 layers), indicating that the growth of the graphene structure was terminated not by blockage of the catalytic template surface, but by the cessation of CVD. This is evidence of a contribution from an autocatalytic growth mechanism; without such a mechanism, no matter how long the CVD could be sustained, we could not expect so many layers. N2 gas adsorption was performed to obtain 142 nm. 2 g -1 The BET surface area and 0.35cm 3 g -1 The BJH porosity. This BJH porosity value is undoubtedly less than the actual specific porosity because the N2 adsorption method cannot measure large pores.

[0389] exist Figure 10 In the highest magnification view shown in C, the layered structure of the coating wall is discernible. It comprises multiple stacks of overlapping z-adjacent graphene regions, confirmed by alternating dark and bright stripes. Each stripe represents a two-dimensional graphene region or a z-space between two z-adjacent regions.

[0390] Care must be taken during HRTEM analysis to avoid confusing the stripes corresponding to the actual locations of graphene layers with those corresponding to the z-spacers between these layers. Depending on the defocus value, the stripes associated with the actual atomic locations can be dark or bright. Regardless of their color, the lines associated with the z-spacers will be the opposite color. Examples of dark or bright stripes associated with graphene layers can be found in the literature. Having solid information about the actual molecular structure is helpful in making a reliable assignment of the exact atomic locations in HRTEM images.

[0391] The presence of the striations indicates that this segment of the coating wall in sample A1 comprises a stacked arrangement of z-adjacent graphene regions. Figure 10 Within the main framework of C, several dark stripes are outlined in yellow. As shown by the yellow outlines, although the z-adjacent stripes appear to be roughly xy-aligned at distances up to several nanometers, the stripes are not parallel throughout the entire coating wall. However, due to the xy alignment of the z-adjacent graphene regions, Figure 10 The walls in C exhibit a nematic arrangement. All layers in the imaged walls exhibit a nematic arrangement.

[0392] The xy arrangement between z-adjacent graphene regions allows for smaller z-spacing and higher density arrangement, which in turn enhances interlayer coupling and vdW cohesion. We consider this to be a desirable characteristic of hierarchical graphene systems, distinct from the low-density, non-hierarchical network architecture exhibited by Schwarz structures. If a reduction in density is desired, this can be achieved by introducing larger-scale porosity patterns (such as the large pores in sample A1) while maintaining a high-density hierarchical organization at smaller scales.

[0393] Another helpful example of columnar permutations is in Figure 11 The image shown is an HRTEM image of a coated wall with nematically aligned layers (from different samples). We include this example here because the stripe lines are clearer in the HRTEM image of this sample. Different segments of the wall are highlighted in yellow. In each highlighted area, the stripe pattern exhibits a nematic alignment with the stated segments of the wall. This is likely due to the conformal growth of the graphene structures on the template surface and then on top of each other.

[0394] Although the layers within the entire sample A1 are arranged in a nematic pattern, they are visually difficult to track. Figure 10 The dark stripes in C exceed several nanometers. An exemplary portion of the coating wall is composed of... Figure 10 The white square marked C indicates that the white square is in Figure 10 The image is magnified in the illustration of C. Although the diffraction contrast and focus of this image are not sharp, the fringe lines are discernible and traceable. Dark fringe lines from the HRTEM photomicrograph are outlined in red. Bright fringe lines from the HRTEM photomicrograph are outlined in solid blue in high-contrast bright areas and in dashed blue in low-contrast bright areas.

[0395] Apart from the z-interval between the red line segments, there seems to be a... Figure 10 The red segments in the magnified inset of C are separated by lateral breaks—that is, the blue outlines. This pattern can be observed throughout the entire HRTEM image of sample A1. If the red outlines in the magnified inset represent the location of graphene regions, then each lateral break in the red outlines indicates an edge. If this interpretation is correct (which we will prove is not), the pervasive presence of this striped pattern throughout the coated wall would suggest that the wall may comprise a vdW assembly of small graphene domains (averaging no greater than 3 nm), since these lateral breaks are so common. Furthermore, if this interpretation is correct, we would have to conclude that the graphene edges of adjacent z-layers are aligned. This could be explained if the edges were caused by breakage; however, this possible explanation is unconvincing given the pervasive presence of the striped pattern throughout the wall.

[0396] The correct (alternative) explanation is the bright stripes (corresponding to...). Figure 10The blue outlines in the enlarged illustration of C indicate the actual atomic positions. The solid blue line in the center of the illustration forms a distinct horizontal "Y" shape, as shown... Figure 10 The horizontal Y in C marks this. This bright Y indicates that the bilayer on the branching side of Y and the monolayer on the stem side of Y are simply different regions of the same ring-connected graphene structure. Additionally, in this case, the bright fringes drawn with dashed blue lines, while having lower diffraction contrast than those drawn with solid blue lines, also indicate the presence of some atoms. These solid lines, along with the dashed blue lines, indicate ring connectivity throughout the magnified region—the opposite of the discontinuity indicated by the red lines.

[0397] This observation has precedent in the anthracite literature. HRTEM striations of anthracite have been analyzed to generate models of structural dislocations in anthracite. Figure 12 A to Figure 12 Figure D is borrowed from this HRTEM analysis. Each figure contains a model representing the structural dislocations found in anthracite, and below the model, a simulated HRTEM stripe pattern. These simulated stripe patterns are consistent with the actual stripe patterns observed in anthracite, thus validating the dislocation model. In each simulated stripe pattern, bright stripes represent graphene regions, and dark stripes represent spaces between layers.

[0398] Figure 12 A is an illustration of edge dislocations borrowed from anthracite literature, where graphene regions are trapped between two z-adjacent regions (one on top and one on the bottom). The edges of the trapped regions represent local ends of a graphene structure, and their members may include sp... 2 Free radicals. In van der Waals assemblages formed primarily by subduction events (characteristic of carbon formed via template-guided CVD), the edges of the subducted region—and the z-adjacent regions trapped within it—together constitute edge dislocations. Simulated HRTEM fringe patterns formed by edge dislocations also exist. Figure 12 As shown in A. The pattern is characterized by bright stripes indicating the location of the intercepted area, which terminate between dark Y-shaped stripes indicating the interlayer spacing.

[0399] Figure 12 B is a diagram of Y-dislocations borrowed from anthracite literature, whereby the Y-dislocations can be considered as... Figure 12 A horizontal Y-shaped structure will be formed when the edge atoms of the truncated graphene region in region A are covalently bonded to the adjacent region in region z. Edge dislocations (e.g.) Figure 12 A) to Y dislocation (e.g.) Figure 12 B) The geological transformation lowers the dislocation energy. This will occur via a radical addition reaction, which produces sp at the junction of the three layers in the Y dislocation. 3Atomic lines. Researchers have shown that the Y dislocations in anthracite evolve in this way.

[0400] Simulated HRTEM stripe patterns formed by Y dislocations in Figure 12 Figure B shows the area below the dislocation. The pattern is... Figure 12 The opposite pattern of the simulated pattern in A—that is, the dark stripes terminate between the bright Y-shaped stripes. The bright Y-shaped stripes represent the location of the Y-shaped graphene structure, a smaller version of which is formed by… Figure 7 The molecular model in D is shown. The simulated stripe pattern looks very similar to Figure 10 The Y shape is depicted in the enlarged illustration of C.

[0401] The geologically formed anthracite network is a natural demonstration of how structural dislocations can generate three-dimensional graphene networks. Virtually all the carbon atoms in anthracite are members of the graphene network generated by these cross-linked dislocations, except for the occasional CH, CH2, or CH3 groups attached to the rings (which NMR has indicated are present in very small amounts in their solid state). It is this cross-linking of the graphene network that gives anthracite its hardness and prevents it from peeling or dissolving. NMR spectroscopy has shown that dodecylation of anthracite affects only the edge atoms of this monomer, where "the graphene layers appear to merge."

[0402] Back Figure 10 The fringe pattern shown in the enlarged illustration of C leads us to the conclusion that this pattern is associated with cross-linked dislocations. The solid blue lines indicate Y-dislocations. Lower-contrast fringes drawn with dashed blue lines may indicate less focused or more disordered Y-dislocations. The red segments represent the spaces between graphene layers. Since Y-dislocations are constructed from diamond-like carbon seams that preserve lateral and vertical ring connectivity, we can conclude that… Figure 10 The enlarged inset of C shows the ring-connected region within the enveloped wall. Furthermore, the prevalence of Y-dislocations like these throughout the wall indicates that the enveloped framework in sample A1 comprises an anthracite network.

[0403] Our comparative analysis of samples A2 and A3 further confirms this. That is, if the encapsulated framework in sample A1 includes vdW assemblages, the significantly superior robustness of the fewer crystalline particles in sample A1 compared to the more crystalline particles in sample A2 (their relative crystallinity was determined by HRTEM, Raman, and XRD analyses) contradicts findings reported in the literature. Researchers have demonstrated that vdW assemblages with smaller graphene domains are more fragile—not more robust—than those with larger, more crystalline domains. For example, “amorphous graphene nanocages” with assemblages having similar morphology to the particles in sample A1 and including small overlapping graphene domains (typically less than 10 nm) are prone to breakage and deformation. Their fragility can be explained by the weakening of vdW interactions between the small graphene domains of these assemblages (which are easily sheared apart). A side-by-side comparison of amorphous graphene nanocages with more crystalline graphene nanocages constructed from larger domains demonstrates the superior cohesiveness of the latter. However, what we actually see is a huge improvement in the mechanical robustness of each particle throughout sample A1 compared to the more fragile nanocrystalline particles found in sample A2.

[0404] Based on this, we can say that, Figure 10 The coating framework in A comprises an average of approximately 18.5 layers (based on the theoretical specific surface area of ​​graphene of 2630 m²). 2 g -1 Divide by the BET surface area of ​​sample A1, which is 142m² 2 g -1 The resulting figures represent the anthracite network. Figure 10 The observable portion of the anthracite network in A comprises nine spherical macroporous subunits. In general, this represents a graphite network with numerous lattice regions located at the vdW contact. A conservative estimate of this region is 48 μm. 2 This is based on the following. First, for this estimate, we ignore... Figure 10 Only the 8th and 9th subunits are partially observable in A. While the average radius of the remaining subunits is difficult to calculate precisely, it is certainly greater than 200 nm (for reference). Figure 10 Spherical #4 in A has a radius of approximately 200 nm (as indicated by the black dashed line), but we use this radius for our conservative estimate. The theoretical surface area of ​​seven spheres with a radius of 200 nm would be approximately 3.5 × 10⁻⁶. 6 nm 2 (that is, 7×4πr) 2 (where r = 200 nm). We note that if the spheres are joined, such as they are in... Figure 10 If it were as shown in A, this would be reduced, so we reduce our theoretical surface area by 25%, resulting in a value of 2.6 × 10⁻⁶. 6 nm2 Finally, based on the estimated average wall thickness of 18.5 layers, we can estimate the total lattice area within the entire wall to be approximately 4.8 × 10⁻⁶. 7 nm 2 (i.e., 18.5 floors × 2.64 × 10) 6 nm 2 ), or 48μm 2 .

[0405] Since the entire lattice area of ​​this network is organized in nematic layers, essentially the entire lattice area undergoes interlayer vdW interactions. For the same reason that crystalline graphene nanocages constructed from large-area domains exhibit better vdW cohesion than amorphous graphene nanocages constructed from small-area domains, we can infer that as we progressively construct larger anthracite networks, we can begin to deduce a considerable contribution of vdW to the system's cohesion. This is one reason why we find anthracite networks more attractive than Schwarz-like graphene networks (as shown in Figure 2) (such as those synthesized on zeolite templates). In the case of a denser hierarchical architecture, shorter, more uniform z-spacings and better vdW cohesion are obtained. The resulting increase in local density can then be offset by introducing larger-scale porosity patterns, such as templated pores within the encapsulated framework.

[0406] More information about the in-frame bonding in sample A1 can be derived from the sample's Raman spectra. Single-point Raman spectra obtained using a 532 nm laser with a power of 2 mW are shown in... Figure 13 As shown in the image. Smoothing was not performed. For reference, the full spectrum is shown in... Figure 13 As shown in the illustration. D u The center of the belt appears to be 1345cm. -1 With 1350cm -1 This is characteristic of 532nm (approximately 2.33eV) excitation. Based on this, compared to the conventional 1585cm⁻¹... -1 In comparison, G u The center of the belt is at 1590cm -1 With 1595cm -1 Between, this instruction sp 2 There is some kind of compressive strain in the bond. Additionally, in D... u With G u There are high Tr between the bands u The peak corresponds to an I value of approximately 0.50. Tru / I Gu The peak intensity ratio indicates the possible presence of a fundamental peak that needs to be checked through a line fit. Peak intensity ratio is less than 1.0.

[0407] Figure 13Another obvious unfitted peak in the middle is D. u With a belt at 1100cm -1 With 1200cm -1 The weak shoulder. This feature is located between 1150 and 1200 cm. -1 D found in the area * The peaks overlap. Researchers in this field have attributed this peak to the sp. of soot-like carbon. 2 Region and SP 3 sp at the transition between regions 2 -sp 3 Key. Therefore, this attribution is related to the sp of the structural diamond-like joint. x The rings are very consistent.

[0408] In order to clarify Figure 13 The basic characteristics of the Raman line shape were determined using the OMNIC peak-splitting software. First, the software was limited to using only two peaks. Figure 14 The graph shows two fitted peaks, the fitted line shape, the actual line shape, and the residuals representing the difference between the fitted and actual line shapes. The residuals at the bottom of the graph indicate the extent and magnitude of the deviation of the fitted line shape from the actual line shape. Flat residuals (considering that noise in the unsmoothed actual line shape will also be reflected in the residuals) indicate that the fitted line shape is good and coincides with the actual line shape. Because there are only two peaks, the fitted line shape is still poor, at approximately 1150 cm⁻¹. -1 With 1650cm -1 Large residuals appear between them. It is noteworthy that these are observed at the peaks, valleys, and at 1150cm. -1 The fit at the left and right shoulders is particularly poor.

[0409] Next, allow the OMNIC peak splitting software to use the third peak, which was manually placed at 1500 cm⁻¹ before rerunning the linear fitting routine. -1 At the starting position. Figure 15 The diagram shows three fitted peaks, the fitted line shape, the actual line shape, and the residuals representing the difference between the fitted and actual line shapes. (At 1566 cm⁻¹) -1 The fitted line shape, incorporating a broad fitted peak, appears significantly better than the fit obtained with only two fitted peaks. However, at 1150 cm⁻¹... -1 With 1200cm -1 Significant residuals still exist between them.

[0410] Next, allow the OMNIC peak splitting software to use the fourth peak, which was manually placed at 1150 cm⁻¹ before rerunning the fitting routine. -1 At the starting position. Figure 16 Four fitted peaks are shown (labeled f-1 to f-4). At 1185 cm⁻¹... -1The fitted line shape, further incorporating a broad fitted peak, appears significantly better than the fitted line shape obtained with two or three fitted peaks. 1185cm -1 The f-1 peak at this point reduces the residuals associated with the shoulder features within this range. Using these four fitting peaks, a satisfactory fitted line shape was obtained.

[0411] Analysis of the four fitted bands shows that the G band (in strain-free sp) 2 In the crystal lattice, typically at approximately 1585 cm⁻¹ -1 (Found at) split into 1596cm -1 The f-4 peak at 1514 cm⁻¹ and the peak at 1514 cm⁻¹ -1 The f-3 peak is located at [location missing]. The f-4 band represents the blueshift mode of the G band. The increased frequencies of these blueshifted phonons are due to some sp[missing information]. 2 -sp 2 Caused by compressive strain in the bond. 1514cm -1 The much broader f-3 peak at [location] coincides with the D” peak found in graphene oxide and indicates a redshift mode in the G band. The lower frequencies of these redshifted phonons are generated by sp[s] in the disordered region of the ring. 2 -sp 2 The strain is caused by the stretching and weakening of the bonds, as described by Ferrari and Robertson. In addition to induced tensile strain, the toroidal disorder in these regions does not allow for a uniform strain field, which broadens the f-3 band. Therefore, from the splitting of the G band into the f-3 and f-4 peaks, we can discern compressive sp. 2 -sp 2 Certain areas of the bond and stretching sp 2 -sp 2 The existence of certain disordered regions of the bond ring.

[0412] No blue shift band like f-4 was observed in graphene oxide. In graphene oxide, the G peak, except for its position at 1585 cm⁻¹, is present. -1 In addition to the normal pattern, a redshift pattern also exists (referred to as the D-peak and characterized as a trough in this paper). This is combined with the lack of oxygen in sample A1 (by... Figure 20 The near-zero mass loss rate below 400°C and the hierarchical architecture of the graphene system confirm that its Raman spectrum is generated by a structure different from that of graphene oxide.

[0413] Figure 17 The f-2 peak in the image indicates that it is located at 1343 cm⁻¹. -1 Slight redshift at D f Peak. Although sp 2 The D band of carbon is dispersed, and the D peak position can change based on excitation, but 1343 cm⁻¹... -1 Slightly lower than that typically associated with sp under 532nm excitation 2Carbon-related D peak position (1350 cm⁻¹) -1 (Left and right). This redshift indicator sp 2 Vibrational Dynamic Density (VDOS) and in sp 3 A potential interpolation in the lower frequency bands discovered in VDOS.

[0414] When strong coupling exists between these phases, VDOS interpolation occurs in the alloy structure. D-band (with sp) 2 Hybridization correlation) and interpolation between lower frequency bands indicate closely approximate sp 3 State and sp 2 Strong coupling of states. These strongly coupled regions are activated throughout the graphene system. 2 Radial breathing pattern (“RBM”) phonons were found within the ring structure. Therefore, even with trace amounts of sp... 3 Carbon states can also be activated by them in much larger sps. 2 The RBM phonons found in the composition were identified in Raman spectroscopy. In other words, the RBM phonons in the grafted monomer originate from sp x sp in the ring 3 Backscattering activation of the state, where sp 2 Xianghe sp 3 The phases are strongly coupled, and therefore the D-band associated with the RBM phonons is interpolated. Conversely, a large number of sp bands, including those between diamond-like joints, are interpolated. 2 layer sp 2 The state is not adjacent to sp 3 The states are not strongly coupled with them, and therefore with sp 2 -sp 2 The vibration-associated G-band was not interpolated. Based on this analysis, Figure 17 The redshift position of f-2 in (i.e., D) f The peak confirmed the observation of ubiquitous Y-dislocations throughout the anthracite network, including sample A1.

[0415] The degree of D-band interpolation is not determined by the sp_s within the graphene system. 3 The score of the state is not determined by sp. 3 The fraction of RBM phonons activated by the state and the fraction of sp 2 The fraction of RBM phonons activated at edge states. If even fewer sp... 2 Edge states, even trace amounts of sp 3 The state can also activate most RBM phonons. This can cause interpolation in the D-band, and the degree of interpolation can be expected to increase with sp. 3 The universality of the increase in state and sp 2The prevalence of edge states decreases and increases. Of course, the corresponding prevalences of these two states are negatively correlated because sp... x The ring is through sp 2 edge state to sp 2 Internal state or sp 3 It is formed by the transformation of state.

[0416] Therefore, the interpolation of band D in sample A1 can be regarded as sp 2 Edge state to sp associated with diamond-like joint 3 Evidence of state transition. 2 Edge state to sp associated with diamond-like joint 3 The state transition also suggests the geological tectonic mechanism behind the formation of the joint, and this causal mechanism will be further explored in conjunction with samples A3 and those involved in study B.

[0417] Beyond the f-2 peak, sp is present in the Raman spectrum. 3 Another possible indication of the state is related to D. u Peak-associated shoulder features. In Figure 13 Appeared at 1100cm -1 With 1200cm -1 Between this shoulder by Figure 16 The broad f-1 peak in the fit is centered at 1185 cm⁻¹. -1 Location. Previous researchers have placed 1150cm. -1 With 1200cm -1 The broad peaks between them belong to sp 2 -sp 3 The bond, and therefore the broad peak will correspond to the transition appearing at the diamond-like carbon seam. To demonstrate that this characteristic is independent of trans-PA, we annealed sample A1 at 1050 °C for 30 minutes. The fitted Raman spectrum of the annealed sample is shown in... Figure 17 The image is shown for comparison. Shoulder feature strength decreased from 1185cm. -1 Slightly offset to 1180cm -1 However, it was not eliminated. This indicates that it is not trans PA. Nevertheless, annealing reduced the area ratio of the f-1 peak (i.e., the ratio of its area to the total area of ​​all four fitted peaks) from 0.16 to 0.11. This reduction indicates sp 2 -sp 3 The reduction in bonding, and the possible sp 3 The content decreased. Therefore, the f-1 peak can also confirm the diamond-like carbon joint in sample A1.

[0418] A review of the literature on anthracite coal indicates that the redshifted D band (unfitted D peak) in the optical Raman spectra of certain grades of natural anthracite coal occasionally appears at 1340 cm⁻¹. -1The following locations were found where, in other less mature or more mature grades, the D-band appears not to have been interpolated. In less mature grades, it can be inferred that this is because the diamond-like carbon (DLC) joints have not yet formed geologically. In more mature grades (e.g., metamorphic anthracite), it can be inferred that the DLC joints have formed and subsequently become unstable, thus eliminating the sp-band. 3 The state and evolution of screw dislocations.

[0419] To the best of our knowledge, the cause of the accidental redshift of the D peak has neither been studied nor attributed to diamond-like carbon seams. In optical Raman spectroscopy, anthracite... The ratio is often below 1.0, as seen in sample A1. Additionally, anthracite typically exhibits a location around 1595 cm⁻¹. -1 With 1605cm -1 The blue shift G peak between, and the fit at 1500 cm⁻¹ -1 Up to 1550cm -1 The broad fundamental peak between these peaks is consistent with the redshift pattern of the G peak. Additionally, some grades of anthracite exhibit a peak at 1100 cm⁻¹. -1 Up to 1200cm -1 The shoulder is within the range. Therefore, the spectrum of sample A1 and its HRTEM stripe pattern are consistent with the synthetic anthracite network.

[0420] Further characterization of the anthracite network in sample A1 was obtained through XRD analysis. XRD analysis was performed on a sample synthesized using a procedure similar to A1 but from magnesium carbonate feedstock powder. This feedstock powder was calcined to obtain MgO powder with template particles indistinguishable from those in sample A1. Therefore, the XRD results from this carbon were analyzed to understand the crystal structure of the anthracite network like that in sample A1. Figure 18 The overall XRD shape is shown. Table 2 below contains XRD peak angles, d-intervals, areas, area percentages (normalized to the area of ​​the main peak at 2θ = 25.044°), and full width at half maximum (FWHM) values ​​(uncorrected instrument broadening):

[0421] Table 2

[0422]

[0423] Three peaks are fitted within the interlayer periodicity range. These three fitted peaks are called peaks I, II, and III, and... Figure 18 Mark it in the middle. Figure 18 It also includes a reference line showing the 2θ values ​​associated with the graphite index. For sample A1, the largest fitted peak, as measured by the area under the peak, is peak II. Peak II achieves its maximum height at 2θ = 25.044°, which corresponds to... The d-interlayer spacing was set. The area under peak II was set to 100% for comparison with other peak areas. The FWHM value of peak II is 5.237°, indicating a relatively wide range of interlayer spacing. The d-interlayer spacing and FWHM value of peak II together indicate that the interlayer spacing in sample A1 is more variable and larger compared to the interlayer spacing in graphitic carbon.

[0424] Peak I has its maximum height at 2θ = 20.995°, which is equivalent to The d-interval. Like peak II, peak I is also very wide, with an FWHM value of 4.865°. The area under peak I is 32% of the area under peak II, making it an important phase for interlayer spacing. The d-spacing is too large to be correlated with the interlayer phases in graphitic carbon. This peak reflects the presence of z-adjacent curved graphene regions with different curvatures. Heterogeneous z-deflection disrupts the uniformity of interlayer spacing and creates expanded spaces between curved regions. This curvature is consistent with anthracite networks.

[0425] Peak III also indicates the presence of a smaller interlayer spacing phase. The maximum height is at 2θ = 30.401° (which is equivalent to...). In the case of a d-spacing, the interlayer spacing represented by peak III is smaller than that of any interlayer phase in graphitic carbon. Like peaks I and II, peak III is broad, with an FWHM value of 8.304°. The area under peak III is 80% of the area under peak II, making it an almost equivalent interlayer spacing phase. No interlayer spacing phase has been found in graphitic carbon. Within the range of d-spacing values, graphite carbon typically has of <002> The d-space value, and none greater than that of graphite. of <100> Other d-spacing values. Heating and compression of glassy carbon leads to sp... 2 The buckling of the region, sp 2 to sp 3 Rehybridization, and interlayer spacing between and sp between 2 / sp 3 Alloy formation. The d-space is... Peak III of sample A1 is consistent with this, thus further confirming the presence of sp in sample A1. 3 The existence of a state.

[0426] Consistent with the blue shift pattern of the G peak in sample A1, its XRD line shape reflects... <100> Compression. Within the intralayer peak range, fitting was performed. <100> The fitted peak has its maximum height at 2θ = 30.401°, which is equivalent to... The d-spacing. The peak is wide, indicating... <100> The range of d-space values ​​is wide. (Compared to graphite) Compared to the d-spacing, of <100> The d-space represents approximately 2% of the compressive strain in the xy plane.

[0427] The thermal oxidation linearity of sample A1 is in Figure 19 The derivative of mass loss of the samples with respect to temperature is plotted. The onset of thermal oxidation in sample A1 occurs between 450°C and 500°C. This is higher than that of sample A3 and roughly the same as that of sample A2. This indicates that the amount of volatile mass in sample A1 is negligible compared to carbon oxide like graphene oxide. The peak mass loss temperature at approximately 608°C is lower than that of sample A2 but higher than that of sample A3. Overall, these results are consistent with the temperatures at which CVD is performed; high-temperature pyrolysis processes generally produce carbon with higher thermal oxidation onset temperatures and higher peak mass losses due to increased crystallinity. The only exception to this trend is the earlier onset of thermal oxidation in sample A2, which can be attributed to the small amount of soot observed in certain regions of the sample. This soot phase is not conformal to the substrate and is likely formed by gas-phase pyrolysis in free space due to the high-temperature pyrolysis in procedure A2. The remainder of sample A2 exhibits higher thermal oxidation stability than the other samples, resulting in the highest peak mass loss temperature among all three samples.

[0428] Figure 20 This is an SEM image of sample A2. Analysis of the image reveals the presence of carbon particles that appear to be fragmented coated frameworks. Similar to sample A1, the templated morphology of the framework is evident, and the coating walls appear to have encapsulated and replicated the template surface. However, unlike sample A1, in many cases, the framework appears broken and deformed. This loss of native morphology confirms a weakened ability of the coating walls to withstand the mechanical stresses encountered during liquid-phase template extraction and drying. Given the mild nature of the extraction procedure (involving gentle agitation and subsequent drying), this fragmentation suggests that the coated framework does not comprise a complete anthracite network, but rather consists of vdW assemblages that can easily break and deform due to shear-related fracture.

[0429] TEM analysis of sample A2 confirmed the deformed and fragmented appearance of the frame in the SEM image. Figure 21 A TEM image revealing the extent of damage that occurred during template extraction. This contrasts with largely intact, undeformed particles (such as...) observed in sample A1. Figure 10 Compared to (as shown in A), the appearance is extremely different. Figure 21 In sample B, it was revealed that the coating wall has a thickness comparable to that of sample A1. The BET specific surface area of ​​sample A2 was measured to be 127 m². 2 g -1 (BET specific surface area of ​​sample A1 (142m²) 2 g -1(Approximately 10% lower), suggesting that the average wall thickness of sample A2 is between 20 and 21 layers—slightly thicker than sample A1. Sample A2's is 0.37 cm. 3 g -1 The BJH specific porosity is also similar to that of sample A1 (0.35 cm⁻¹). 3 g -1 Although we again note that this measurement underestimates the contribution of larger pores.

[0430] exist Figure 21 In sample C, striations associated with the layered architecture can be observed. Regardless of the long-range curvature of the coating walls, both dark and bright striations are approximately linear. This indicates a reduction in ring disorder and Gaussian curvature in these graphene regions compared to the region observed in sample A1. Figure 21 As shown by the red lines in C, the stripe lines are essentially parallel, so we can describe these layers as nematically arranged. While several potential examples of stripe patterns associated with cross-linked dislocations can be identified, these examples are considerably rarer compared to those in sample A1. Although there are occasional cross-linked dislocations in these encapsulated bodies, they are insufficient to form anthracite networks.

[0431] More information about the bonding structure of sample A2 can be derived from its Raman spectrum. Single-point Raman spectra obtained using a 532 nm laser with a power of 2 mW are shown in the image. Figure 22 As shown in the image. Smoothing was not performed. The three main features of the line are approximately 1349 cm. -1 D at the location u Peak, approximately 1587cm -1 G at the location u Peak and approximately 2700cm -1 2D at the location u peak.

[0432] Compared to sample A1, sample A2 has an intensity Tr u The features are much lower, I Tru / I Gu The ratio is less than 0.15. This is consistent with the small contribution of the potential redshift mode of the G peak and the absence of ring disorder-induced tensile strain. The lack of ring disorder and associated tensile strain is related to the fact that... Figure 21 The smaller Gaussian curvatures observed in C are very consistent. Additionally, G... u The peak is at 1587cm -1 The natural position at this point indicates that the compressed region present in sample A1 does not exist. 2D u The prominent presence of peaks indicates the mixed-layer stacking arrangement of hexagonal tiling layers in sample A2.

[0433] The average D of sample A1 u Compared to the peak, the average D of sample A2 uThe peak exhibits higher intensity, with an average I Du / I Gu The ratio is greater than 1.0. This includes 2D. u The appearance of peaks (and average I) 2Du / I Gu The ratio of 0.265 reflects the increased crystalline order in sample A2 compared to sample A1. Although the increase in D band intensity in the crystalline carbon spectrum corresponds to a decrease in crystallinity (e.g., in the amorphization of graphite to nanocrystalline graphite), sample A1 is nanocrystalline, so its higher D band intensity indicates increased crystalline order compared to sample A2.

[0434] G u The peak is at approximately 1620 cm. -1 There is a slight asymmetry at the shoulders. This stems from the height of 1620cm. -1 The fundamental peak at point D', the fundamental peak due to the sp of sample A2 2 The high density of the edge states makes it more noticeable. 2 The prevalence of edge states also shifted from the center at 1349cm. -1 Narrow D at the location u Peak indication. This D-band appears to be unaffected by any low-frequency sp. 3 Significant interpolation indicates that most RBM phonons are sp 2 Edge-state activation is not caused by sp associated with diamond-like joints. 3 The state is active. D was observed in sample A1. * The peak is either nonexistent or negligible.

[0435] Table 3 below contains the XRD peak angles, d-intervals, areas, area percentages (normalized to the area under the main peak at 2θ = 25.8319°), and FWHM values ​​(uncorrected instrument broadening) of samples synthesized using a procedure similar to A2 but from magnesium carbonate feedstock powder. This powder was calcined to obtain MgO powder indistinguishable from the template particles of sample A2. Therefore, the XRD results from this carbon were analyzed to understand the crystal structure of assemblages like those in sample A2.

[0436] Table 3

[0437]

[0438] Three peaks are fitted within the interlayer periodicity. These three fitted peaks are named peaks I, II, and III, with ascending numbers corresponding to the ascending 2θ values ​​at which the peaks obtain their maximum intensity. For example, the maximum fitted peak, measured by the area under the peak, is peak II, which obtains its maximum height at 2θ = 25.8319°, and corresponds to a spacing of d. The area under peak II was set to 100%. The d-spacing value of peak II is related to that of the mixed-layer graphitic carbon. <002> The d-spacing is consistent, and the peak is quite sharp compared to peak II of sample A1.

[0439] Peak I has its maximum height at 2θ = 22.9703°, which is equivalent to The d-interval—from the peak I of sample A1 The corresponding d-interval shrinkage. The area under peak I is only 13% of the area under peak II, making it a significant but smaller phase, while in sample A1, the area of ​​phase I is 32% of the area of ​​phase II. The presence of peak I may reflect a larger z-interval at the edge dislocation, or the reduced but not eliminated presence of non-hexagonal rings. Large irregularities. <002> The reduced spacing of d is again consistent with the appearance of the more arranged planar stripes in sample A2, such as Figure 21 As shown in C.

[0440] Peak III indicates the presence of a small amount of interlayer spacing contraction phase. The maximum height is at 2θ = 31.2063° (which is equivalent to...). In the case of a d-spacing, the interlayer spacing represented by peak III is significantly smaller than any interlayer spacing in graphitic carbon. Peak III is also very broad, with an FWHM value of 10.33°. The area under peak III is only 5.1% of the area under peak II, making it a rather negligible phase. This is consistent with the sparseness of Y dislocations observed in sample A2.

[0441] Finally, the intralayer periodicity at 2θ = 42.6906° corresponds to of <100> d-space, which is close to The graphite d-spacing. This confirms the presence of G. u The peak is at 1587cm -1 The lack of compressive strain reflected in the natural position of the dislocation suggests that compressive strain is somehow related to the formation of crosslinked dislocations and the xy intervals in which they occur.

[0442] The thermal oxidation linearity of sample A2 is in Figure 19 The derivative of mass loss of the samples with respect to temperature is plotted. Thermal oxidation of sample A2 begins between 450°C and 500°C, which is higher than that of sample A3 and roughly the same as that of sample A1. The peak mass loss temperature of sample A2 at 650°C is higher than that of samples A1 and A3, reflecting the increased stability of its nanocrystalline graphite structure. The larger temperature range at which sample A2 is thermally oxidized corresponds to the presence of easily oxidizable soot that causes the earlier initiation of thermal oxidation.

[0443] Further practical evidence of the deteriorated mechanical properties in sample A2 compared to sample A1 was obtained through a uniaxial compression test. In this test, the powders of samples A1 and A2 were each uniaxially compressed to the same pressure. After compression, sample A1 retained its powder form, indicating insufficient compaction, while the powder of sample A2 was compacted into firm, single flakes.

[0444] Perform SEM to better understand the compressed powder. Figure 23 This is a SEM image of the compressed sample A1 coated framework. It can be observed that the frameworks retain their porous morphology. While fractures of the coating walls are observed in many particles, other coating walls exhibit linear features not present before compression. These linear features... Figure 23 The figures are shown in the figure and enlarged in the illustration. In the illustration, the inward buckling of the coating walls can be observed, forming internal folds that produce linear surface features. Many compressed sample A1 particles exhibit localized buckling, indicating that their coating walls are capable of localized bending. The retention of the framework's porous morphology indicates the walls' ability to resist inelastic shear yielding and store elastic potential energy, thus rebounding upon release of uniaxial compression. This elasticity prevents the framework from irreversibly compressing into paper-like particles due to the anthracite network within the walls.

[0445] In comparison, Figure 24 This is a SEM image of the coated framework of sample A2 after compression. The porous morphology of the framework in sample A2 has been disrupted. The resulting sheet-like layered structure is consistent with the observed trend of increased plastic deformation and fragmentation of these frameworks during liquid-phase treatment and drying. During compression, the layers within the coated wall are able to shear due to the lack of anthracite network. The loss of porosity and compaction into a laminated structure are the causes of the granular structure, which cannot rebound upon release of uniaxial compression due to the lack of stored elastic potential energy. Therefore, the lack of anthracite network in the wall hinders the ability of the coated framework in sample A1 to rebound.

[0446] Figure 25 A is the SEM image of sample A3. Like the particles in sample A1, the encapsulated framework in sample A3 retains its original pore wall morphology with little sign of deformation. This morphology reflects the template, which comprises partially sintered powder of bonded polyhedral MgO crystals, such as... Figure 26 As shown, the joint subunits of the enveloped framework have large, flat facets and appear more polyhedral than the subunits in sample A1. Figure 25 In the SEM micrograph of A, it is unclear where a single frame begins or ends, or how many different frames may exist in this image.

[0447] Compared to the encapsulated walls in samples A1 and A2, which exhibit a consistent appearance, the walls in sample A3 have both transparent and opaque areas. The transparent areas exist within the flat facets of the frame and, at first glance, appear to be holes in the encapsulated walls. Figure 25 B is Figure 25 An enlarged view of the polyhedral enclosed body present in A. Two transparent areas (“windows”) are circled and outlined in yellow. The windows are located in the central region of the flat facets, as shown... Figure 25 Marked in B, these are surrounded by narrow, more electronically opaque strips around the perimeter of the facets. These strips are referred to as "borders" in this document because they give the windows a framed appearance, such as... Figure 25 As shown in B. The border on the facet is usually close to the edge of the facet, but occasional, more electronically opaque tendrils can be observed extending inward.

[0448] like Figure 25 As shown by the yellow arrow in C, the border surrounding the window typically extends across the window to the opposite side border, as if the border were attached to a transparent surface. Figure 25 In the facet shown by C, and in many other easily identifiable cases, the gentle inward (i.e., toward the interior of the unit cell) curvature of the border can be extrapolated to extend across the micro-recessed transparent surface. This slight concavity is indicated by the curvature of the yellow arrow. This is the first indication that the window is not a physical aperture in the encapsulated wall.

[0449] If there were no actual transparent surface to guide the frame, we would expect to see it irregularly bending, abrading, or curling due to the mechanical stress of template removal and drying. However, if the frame is supported by transparent regions (like connective tissue) extending across the facets of the wall, these irregularities would not be expected. Instead, it would indicate the geometry of the transparent surface, which might be expected to be slightly concave due to the inward pull of retreating water during the frame's evaporative drying. In fact, this is the overall appearance of the frame. The conclusion of the SEM analysis is that the window observed in sample A3 is not a hole, but rather a more electronically transparent phase of the wall.

[0450] Previous researchers have observed a phase transition in carbon from the edges of flat facets to the central regions of the facets. When performing CVD growth of coated frameworks on NaCl cubes, distinct phases of the walls were identified at the edges and corners of the NaCl facets (where nucleation occurs due to localized melting of NaCl in these regions). Based on Raman analysis, these regions comprise multilayered vdW assemblages of small graphene domains. A second phase, consisting of larger, more crystalline domains within the coated walls, was found in the central regions of each facet (i.e., regions with less melting and nucleation). These coated walls fractured during template dissolution and drying, producing small flake fragments. This degradation of the framework contrasts with the integrity of the coated framework in sample A3, in which no observable flake fragments were observed in the dried carbon powder. The observation that the windows in sample A3 did not break and become independent flake particles is a strong indication that the walls in sample A3 comprise an anthracite network rather than vdW assemblages.

[0451] Figure 27 A is an HRTEM image of sample A3, which shows the overall microstructure of the sample. Figure 27 The large-pore subunits of the encapsulated framework shown in Figure A are cubic, and the yellow dashed lines are used to facilitate visualization of their cubic shape. More electron-transparent windows on the flat facets of the subunits... Figure 27 A is circled in yellow. Sintering of the MgO template crystal imparts intracellular channels that can be observed between subunits when the template is removed.

[0452] The coating walls in sample A3 are slightly thinner than those in samples A1 and A2. Consistent with this, sample A3 has a higher BET specific surface area of ​​328 m². 2 g -1 This BET measurement suggests an average wall thickness of approximately 8 layers (2630m). 2 g -1 / 328m 2 g -1 =8.0). The cross-section of the coated walls shows that their thickness is fairly uniform and does not exhibit any discontinuities, even in the central region of the flat facets. This is in Figure 27 As shown in Figure C, the cross-section of the cell wall spanning several flat facets (indicated by the yellow dashed rectangles) has a uniform and uninterrupted thickness. This is confirmed by observing the numerous facets from many different angles, and is further indication that the window is not a hole but simply a transparent area encasing the wall.

[0453] Similar to sample A1, sample A3 exhibits numerous Y dislocations. Typical fringe patterns obtained from sample A3 and associated with Y dislocations are shown in... Figure 27 The enlarged illustration of B shows the prevalence of Y dislocations, another indication of the anthracite network responsible for the robustness of the framework in sample A3. Furthermore, like the layering within the walls of sample A1, the layering within the walls of sample A3 exhibits a nematic arrangement. However, the different striations in sample A3 are more difficult to visually trace at any distance greater than 1–2 nm, suggesting a more highly cross-linked anthracite network.

[0454] These observations were confirmed by the Raman spectrum of sample A3. Single-point Raman spectra were obtained using a 532 nm laser with a power of 2 mW. Figure 28 As shown in the image. Smoothing was not performed. For reference, the full spectrum is shown in... Figure 28 As shown in the illustration. The overall Raman shape of sample A3 looks similar to that of sample A1 and anthracite. 2D does not exist. t Peak. D u The center of the peak is at approximately 1340 cm. -1 At this location, more D-band interpolation is reflected than observed in sample A1 (D of A1).u The center of the peak is at 1345 and 1350 cm. -1 (between). This increased interpolation of the D-band reflects the effect of sp. 3 State activation comparison by sp 2 The prevalence of RBM phonons activated at edge states increases. Similar to sample A1, sample A3 has phonons with a frequency between 1150 cm⁻¹. -1 With 1200cm -1 The shoulder between, its indication and in sp x The transition consistency of the base D at the diamond-like carbon joint * Peak. This shoulder is at Figure 28 Mark it in the middle.

[0455] Similarly, sample A3 exhibits a relatively sharp blue shift G, similar to sample A1. u Peak (at 1585cm) -1 The usual G peak position is at Figure 28 (Marked with dashed lines in the middle). This blue shift pattern suggests compressive strain. Compared to sample A1, sample A2 exhibits a slightly lower valley. However, the valley is still high enough to indicate the presence of a broad fundamental peak. We again attribute it to the redshift pattern of the G-band, which is associated with the presence of the ring disorder region.

[0456] A peak intensity ratio of approximately 0.77 indicates a lower D in sample A3 compared to sample A1. u Peak intensity. (D) u This downward trend in peak intensity (A2>A1>A3) is positively correlated with CVD temperature (1050℃>750℃>650℃) and also with D-band interpolation (i.e., with the peak intensity determined by sp...). 3 The prevalence of increased RBM phonons in carbon-activated carbon is positively correlated with this. This decrease in D in disordered carbon... u Peak intensity can be attributed to sp 2 Gradual loss of the ring structure; in the case of sample A3, this is in sp 2 Ring sp x This occurs during ring replacement. The strength of the D-band decreases with increasing diamond-like carbon (DLC) seam density. Therefore, this is consistent with the appearance of the more cross-linked anthracite network in the HRTEM image of sample A3.

[0457] Based on our characterization of samples A1, A2, and A3, we can infer the geological tectonic path along which diamond-like joints formed during growth. We begin this discussion with the observation that the window regions of the coating walls are electronically transparent, while the surrounding borders and the curved regions of the coating walls are not. We then connect this to the analysis of nucleation and growth of the primordial domains on the template surface. Finally, we model the geological encounters between these primordial domains and demonstrate how diamond-like joints evolve from these encounters under appropriate conditions.

[0458] The non-uniformity of electron transparency in sample A3, such as Figure 25 As shown, this is due to the different charging behaviors in different regions of the coating wall. During imaging, more charging occurs in the more electrically insulating regions of the coating wall. This charging behavior is clearly related to the geometry of the template surface. More conductive windows and atomically flat template surfaces (such as...) Figure 26 The small facets marked in the middle (where nucleation of the original domain is rare or nonexistent) are associated with areas of lower conductivity in the coating walls, such as the frames and circular regions, which are associated with more defects on the template surface (where nucleation of the original domain is relatively dense).

[0459] Next, we recall that D based on sample A3 u Peak interpolation, a large portion of the RBM phonons in sample A3 are composed of sp 3 The state is activated, and we associate this state with diamond-like carbon (DLC) joints throughout the entire anthracite network. The DLC joint density is higher in the walls and therefore... 3 In regions with higher state density, we expect enhanced charging due to discontinuities in the π-cloud (through which conductivity occurs). The diamond-like carbon seam density in the walls is lower, and therefore sp... 3 In regions with lower state density, we would expect less charging to occur. Combining these observations, it seems that regions of the coated wall associated with higher nucleation density appear to be charged more, and we attribute this to the sp associated with diamond-like joints. 3 A higher density of states. We further study the sp in these regions. 3 The higher density of the state and diamond-like carbon (DLC) seams is attributed to grafting that occurs at the geological interface of the primordial domains growing on the common substrate surface. Dense local nucleation leads to the proliferation of the primordial domains, resulting in increased geological interactions, more grafting, and therefore more sp. 3 State and diamond-like joint.

[0460] Next, we analyze the geological encounters between these primordial domains. The ring disordered lattices possess non-zero Gaussian curvature, and their edges exhibit a wavy geometry determined by the local lattice curvature. The ring disorder of primordial domains grown by pyrolysis at temperatures below 900°C has been demonstrated in several examples in the prior art (including ring disordered domains in single-crystal MgO). <100> wafers and single-crystal germanium <100> (Growth on a wafer) confirms this. When two such primordial domains are grown on a common substrate surface, a geological encounter can occur between their edges. Due to the different phases of the local lattice curvature and wavy edges of the domains, this geological encounter forms a random, discontinuous geological interface between nearby edge fragments. Adding to this complexity is that the edges of the primordial domains can be conceptualized as free radical fluids that are constantly rearranging themselves. The discontinuity of the interface (where edge atoms of one primordial domain are inconsistently above, below, or at the same level as edge atoms of another domain) prevents the formation of a geological interface through simple dive or sp. 2 The grafting process is analyzed.

[0461] exist Figures 29 to 36 In the middle, we provide sp at the interface of discontinuous geological structures. 2 and sp 3 How can grafting lead to sp. 3 The gradual illustration of states and diamond-like joints, as observed in sample A3, reveals that these states and joints induce localized charging in the enveloped regions associated with dense geological tectonic activity. Several comments are offered in turn regarding the molecular models presented in these figures, and also regarding all other molecular models that run throughout the remainder of this disclosure. First, while we must represent these systems statically, our molecular models should be understood as static representations of dynamic, self-rearranged structures. Second, all such illustrations made using molecular models constructed with Avogadro 1.2.0 software should be considered as only rough geometric approximations of the actual systems. They are intended to provide a useful visual illustration of the phenomena described herein. Third, although we do not show the substrate, the pyrolytic growth process of primary concern in this disclosure is substrate-guided, and the absence of the substrate in the system is not intended to imply its absence. Fourth, we do not represent hydrogen atoms in these illustrations because we are primarily concerned with the evolution of graphene structures, which, by definition, do not include hydrogen. However, in practice, we understand that the hydrogenation and dehydrogenation of these graphene structures theoretically occur dynamically throughout the pyrolytic carbon formation process. Fifth, we provide multiple perspective views to facilitate visual examination and understanding of these systems in three dimensions. Sixth, while we frequently indicate the sequential evolution of the systems under consideration for illustrative purposes, we do not intend to suggest that the order shown in the figures is strict or general. Seventh, we intend to demonstrate how sp. 2 Grafting and sp 3Graft-derived diamond-like joints, chiral pillars, and screw dislocations. We attempt to model how this occurs using the simplest possible models to convey the basic concepts.

[0462] exist Figure 29 The illustration shows a discontinuous geological interface. The interface is formed by the geological encounter between two edge segments (E1 and E2), each belonging to a different cyclic disordered graphene structure (G1 and G2, respectively). These edge segments and graphene structures... Figure 29 They are marked in the diagram. The geological interface between them is described as the E1-E2 interface. We can consider G1 and G2 as primordial domains of nucleation on a common substrate surface.

[0463] Figure 29 The E1-E2 geological interface includes a zigzag-zigzag interface—that is, where both participating edge segments are at a zigzag orientation. This configuration can evolve with the rearrangement of the growing graphene structure itself to align with the growth of free radical condensates. From Figure 29 In the H2 perspective view, we can see that both the original domains G1 and G2 are curved. Therefore, their edges have a wavy geometry. The discontinuity of the z-rotation at the geological interface creates three distinct interface zones—two offset zones located on either side of the E1-E2 geological interface (labeled "Offset Zone I" and "Offset Zone II"), and the horizontal zone in between. These geological zones... Figure 29 Mark it in the middle.

[0464] The vertical offset within the offset region prevents relative edge atoms from forming sp with their counterparts without severe lattice distortion or subduction. 2 -sp 2 Bonding. It is also unfavorable for one edge to be subducted by another. In the offset region, under suitable pyrolysis conditions, edge atoms can undergo sp... 2 to sp 3 Rehybridization and formation of sp 3 -sp 3 Bond lines, which join the original domains together, are edge-to-edge. The sp lines that form the bonds in the offset region... 3 The formation of states is described in this paper as "sp 3 graft".

[0465] In the horizontal region, the vertical offset between the two edges is small enough, and relative to sp 2 The two p atoms of the edge atom z The orbitals are sufficiently aligned to allow π bonds to form between edge atoms. Within these regions, under suitable pyrolysis conditions, edge atoms can form sp bonds with each other. 2 -sp2 The lines of the bond. This is similar to the sp observed between ring-ordered domains in the prior art. 2 Grafting is simply sp at discontinuous interfaces. 2 Grafting is limited to the horizontal region.

[0466] exist Figure 30 In the diagram, the system has passed the sp in the horizontal area. 2 Grafting modification is predicated on the relative sp of E1 and E2. 2 Minimum vertical offset between atomic members and their two p z The orbitals are fully aligned. The resulting two sp... 2 -sp 2 The bonds form a new 6-membered ring, which connects the original domains E1 and E2. These original domains then aggregate to form a new graphene structure designated G3. The new graphene structure G3... Figure 30 Marked in the vertical perspective diagram. New SP 2 The formation of rings, such as Figure 30 This indicates that the resulting G3 domain exhibits a certain degree of permutation distortion. It is noteworthy that, in some cases, grafting events can distort the original interface, causing the interface region to dynamically expand or shrink.

[0467] exist Figure 31 In the diagram, Figure 30 The graphene structure G3 shown has passed through two offset regions. 3 Grafting for structural improvement presupposes a substantial vertical offset between the edge atoms in these regions. This involves the sp... of 10 B3 edge atoms. 2 to sp 3 Rehybridization and 5 sp 3 -sp 3 Key (in) Figure 31 The associated bonds (highlighted in red) are organized into two different sp... 3 -sp 3 Key lines. From the vertical perspective view, we can see 5 sps. 3 -sp 3 The formation of bonds across the E1-E2 geological tectonic interface resulted in the formation of 5 new sp bonds. x Ring. From the H1 perspective view, we can see 2 sps. 3 -sp 3 The bond lines (bond line I corresponding to offset region I and bond line II corresponding to offset region II) have opposite orientations.

[0468] via sp 2 Grafting and sp 3 The six loops formed by grafting Figure 31 Marked in the middle. In the 6-element sp associated with the horizontal region.2 On each side of the ring (labeled R3), there exists a 6-element sp. x Ring (marked as R) 2-C and R 4-C ). In R 2-C and R 4-C Of the two, the 6 yuan SP x The ring contains a chiral chain. The chiral chain contains sp x The four sps of the ring 2 Atoms, and at each end by two sp atoms of a ring. 3 Hybridization terminates. These sp atoms... 3 site via sp 3 -sp 3 The bonds bond together, thus closing the loop. This is in Figure 31 The H2 perspective diagram illustrates that R 2-C The chiral chain is highlighted with a blue arrow, the direction of which coincides with the direction of increasing height in the z-direction. The sp within the chiral chain... 2 Atoms are represented by black circles, while sp at the end of the chiral chain 3 Atoms are represented as black and white circles. These two terminals (sp) 2 sp between atoms 3 -sp 3 The keys are highlighted in red. These two sps contain chiral segments. x The ring represents a chiral ring, and in Figure 31 The symbol is R 2-C and R 4-C .

[0469] Due to the chiral geometry imposed by their chiral chains, sp x Ring R 2-C and R 4-C Indicates a chiral ring. Figure 31 These two chiral rings form at the transition between the horizontal region and the laterally adjacent offset region. It is this transition of geological tectonic zones and the associated changes in edge height that form the chiral chain. Therefore, chiral rings form at the transition of interface zones, and their chirality is determined by the transition of the zone where they form.

[0470] exist Figure 31 In the middle, the other 3 sp x The rings (R1, R5, and R6) have a chair-like configuration. They exhibit two different orientations, such as... Figure 31The H1 perspective diagram illustrates this. Each orientation represents a point reflection in the xy plane of another orientation. These orientations are predetermined based on the geometry of the offset regions that form R1, R5, and R6. R1 is formed by grafting across offset region I, where E2 rises above E1; therefore, R1 rises to the height initially located on the E2 side. On the other hand, R5 and R6 are formed by grafting across offset region II, where E1 rises above E2; therefore, R5 and R6 initially located at the height on the E1 side. This reversal of edge heights is what these sp... x Point reflection orientation of the ring (and two sp) 3 -sp 3 The reason for the opposite orientation of the bond lines.

[0471] The reversal of the edge height between the two offset regions also affects the chiral ring R formed at the transition point between the two regions on either side of the horizontal region. 2-C and R 4-C Apply the same chirality. If the edge height is not reversed between offset region I and offset region II, then R 2-C and R 4-C It will have opposite chirality. This alternative case is in Figure 60 As shown in screen II.

[0472] Follow the sp within the offset region 3 graft, Figure 31 sp in 3 The atom is only triple-coordinated and represents a tertiary free radical. (and) Figure 31 5 sps 3 -sp 3 The bonds associated with these bonds are the five sp bonds representing the elevated tertiary free radicals. 3 Atoms. These elevated tertiary free radicals in Figure 31 They are circled in the H1 perspective diagram and indicated with black and white circles in the H2 perspective diagram. Each of these five elevated free radicals has unpaired electrons extending into the z-space above.

[0473] Figure 31 The graphene structure G3 shown represents the "substrate"—that is, the base layer formed during pyrolytic growth through grafting of the original domains. After grafting, the substrate can exhibit tertiary radical sites extending into the z-space, such as... Figure 31 Those shown. The formation of the substrate eliminates the sp associated with the broken original domain. 2 Edge state. In the region of the base corresponding to the offset region, the sp of the original domain 2 Edge atoms transform into sp 3 Internal atoms. In the region of the substrate corresponding to the horizontal region, sp 2 Edge atoms are sp 2Internal atomic substitutions. These substitutions alter the Raman spectrum of the substrate—specifically, the sp... of the active RMB phonons. 2 Fewer edge atoms, and sp 3 The situation has escalated.

[0474] exist Figure 32 In the diagram, radical addition reactions have occurred at the five elevated tertiary radicals of substrate G3, thereby adding five z-adjacent sp radicals. 3 Carbon atoms are bonded to G3. 5 z-adjacent sp atoms 3 Atoms in Figure 32 The middle part is represented by black and white circles. Their addition forms sp above the basal layer level (i.e., bone lines I and II). 3 -sp 3 The second level of the bond line. These new sp... 3 -sp 3 Key in Figure 32 The center is highlighted in red.

[0475] exist Figure 33 In the illustration, the continuous radical addition reaction above the substrate leads to 9 sp... 3 Atoms (made of) Figure 33 (The nine black and white circles in the V and H2 perspective views indicate) and three sp... 2 Atoms (made of) Figure 33 The addition (indicated by the three solid black circles in the V and H2 perspective views) results in sp. These atomic additions lead to sp. 3 -sp 3 sp is formed above the second level of the bond line 3 -sp 3 The third level of the bond line (in) Figure 33 (Highlighted in red in the V and H2 perspective diagrams). We now notice that sp 3 -sp 3 The orientation of each successive level of the bond line is a point reflection of the orientation in the level above or below.

[0476] The addition reaction also resulted in the formation of three additional 6-membered sps. x Rings (marked as R7, R8, and R9, and in) Figure 33 (marked in the middle), they are respectively associated with 3 sps x Rings R1, R5, and R6z are adjacent. Because of the new sp... x Each in the ring and its underlying base in sp x Rings share more than one atomic member, therefore these sp x Each in the ring and its sp below it x The rings are adjacent. The new amplified graphene structure is achieved through these 3 sp... xIt is formed by the vertical addition of rings; we can designate this new graphene structure as G4.

[0477] Like the sp below them x Rings R1, R5, and R6, sp x Rings R7, R8, and R9 have a chair-like configuration and each has a sp representing the area below it. x Point reflection of the ring. z adjacent sp x Rings R1 and R7 together form a first-class diamond joint, and the other four sp... x Rings (R5, R6, R8, and R9) constitute a second type of diamond joint, wherein two diamond joints (in) Figure 33 (Isolated in the enlarged inset of the H1 perspective view) nascent Y-dislocations oriented in opposite directions are formed (as indicated by the gray shading in the enlarged inset of the H1 perspective view). The diamond-like joint terminates internally at a chiral ring (or, where the joint extends vertically, at a chiral pillar). Figure 33 In the H2 perspective image, we can see that the chiral ring R 2-C and R 4-C Located at the inner end of the diamond-like carbon joint.

[0478] exist Figure 34 In the illustration, the continuous radical addition reaction above the substrate leads to 9 sp... 3 Atoms (made of) Figure 34 (The 9 black and white circles in the V and H2 perspective views indicate) and 18 sp 2 Atoms (made of) Figure 34 The addition (indicated by the 22 solid black circles in the V and H2 perspective view). Simultaneously, some primary carbon atoms from the previous stage have become triple-coordinated sp atoms. 2 Atoms. In this diagram, we begin to see a sustained radical addition reaction driving the vertical sp atoms above the substrate. 3 Growth and lateral sp 2 Both grow. 3 -sp 3 sp above the third level of the key 3 -sp 3 The fourth level of the bond line is in Figure 33 The V and H2 perspective diagrams are highlighted in red.

[0479] exist Figure 34 Located in 3 sp x Directly above and adjacent to rings R7, R8, and R9 are three new 6-element sps. x Ring, marked R 10 R 13 and R 14 Located in the chiral ring R 2-CThe one above is the new 6-element chiral ring, marked with R. 11-C This novice chiral ring is marked in the H2 perspective view. To facilitate visual identification of the z-adjacent chiral ring R... 2-C and R 11-C They are isolated in the enlarged inset of the H2 perspective view. 2-C and R 11-C The atomic members are labeled as 1, 2, 3, ..., 6 and 7, 8, 9, ..., 12, respectively, where sp 2 Members are depicted in black numbers and sp 3 Members are depicted using gray numbers. From this, we can see that, like R... 2-C R 11-C Contains a chiral chain. A chiral chain with two loops in... Figure 34 The enlarged inset of the H2 perspective view is highlighted by blue arrows, the direction of which coincides with the increase in height in the z-direction. The chiral chain of R2-C comprises atoms 1 to 6, wherein atoms 1 and 6 are characterized by sp... 3 -sp 3 sp keys connected to each other 3 Atom. R 11-C The chiral chain comprises atoms 7 to 12, wherein the terminal atoms 7 and 12 include atoms connected by sp... 3 -sp 3 sp keys connected to each other 3 atom.

[0480] These two adjacent z-rings are connected via sp 3 -sp 3 The z-direction chain of the bond (including sps labeled 1, 6, 7, and 12) 3 Member atoms) are connected. Chiral rings and sp 3 -sp 3 The z-direction chains of the bond include chiral pillars. Like chiral rings, chiral pillars exist at the inner ends of diamond-like joints in anthracite networks. The basic structure of chiral pillars can be compared... Figure 34 Enlarged illustration of the H2 perspective view in the figure (where R 2-C -R 11-C (The chiral column is isolated) and Figure 37 The diagram in B illustrates this. Within the chiral column are sp atoms, from 1 to 12. 2 and sp 3 a helical one-dimensional chain of atoms (i.e., "sp") x Spiral). x The basic structure of the spiral is Figure 37 The diagram in C illustrates this.

[0481] exist Figure 35 In the illustration, continuous growth above the basal layer resulted in 32 new sps.2 Atoms (in) Figure 35 The addition (indicated by 32 solid black circles in the perspective diagrams of V and H2) is shown. Simultaneously, some primary carbon atoms from the previous stage have become triple-coordinated sp atoms. 2 Atoms. In this illustration, we see that the rings above the substrate have coalesced into a second core layer with a substantially xy-aligned configuration with the substrate and zigzag edge segments substantially parallel to the original geological interface. Further sp 2 Growth can proceed laterally from this higher-level nucleus, such as... Figure 35 As indicated by the black arrow in the H1 perspective view. From Figure 35 In the vertical perspective view, we can see that the second layer is slightly twisted relative to the first layer. This is called Eshelby torsion and is caused by chiral defects such as chiral columns.

[0482] exist Figure 35 The continuous growth reflected in the R-shaped chiral rings of the basal layer has already been observed. 4-C Another chiral ring R is formed above. 12-C .like Figure 35 As shown in the enlarged inset of the H2 perspective view, the two z-adjacent chiral rings are connected by sp 3 -sp 3 The z-direction chain of the bond connects to form a second chiral column (and within it is a second sp). x (Helix). Due to the basal ring R 2-C and R 4-C The common chirality of chiral chains in R 2-C and R 4-C The two chiral columns formed above also share a common chirality. This common chirality increases the angle of Eshelby torsion.

[0483] Figure 35 The multilayer graphene system shown is classified as anthracite network in this paper. This is achieved through Y dislocations and sp... x The chiral pillars with ring structures undergo lateral and vertical crosslinking, and the entire anthracite network comprises individual ring-connected graphene structures, which are described in this paper as "sp". x "Network." We can begin to see that, with sp x The growth of the network, sp 3 The situation continues to escalate.

[0484] exist Figure 36 In the illustration, the continuous growth above the original G3 substrate has already given sp x A third layer was added to the network. As shown in the vertical perspective view, the third layer exhibits the same Eshelby twist as the second layer. As long as the chiral columns continue to propagate vertically, each higher layer formed will be rotationally misaligned with its z-adjacent layer above or below it. Figure 37 A (which is from) Figure 37 In a magnified view of the H2 perspective (or a similar view to the previous one), we can see that chiral columns continue in each higher-level region. Figure 37 In diagram A, the chiral chains within the chiral rings are highlighted in blue, while the sp chains connecting adjacent chiral rings (z-axis) are shown in blue. 3 -sp 3 The z-direction chains of the bond are highlighted in red. A simplified representation of each chiral post of a z-adjacent chiral ring is shown in... Figure 37 As shown in B. Each of these chiral columns contains sp... x Spiral in Figure 37 It is isolated from C.

[0485] exist Figure 36 In the image, we can see that the continued growth above the original G3 substrate has produced two distinct diamond-like carbon (DLC) seams. These seams include four z-adjacent splines in a chair conformation. x A seam of the two-dimensional strip of the ring is bolded in the enlarged illustration of the H1 perspective view. It includes 10 z-adjacent sps in a chair-like configuration. x Another seam of the two-dimensional sheet of the ring is in Figure 36 Another enlarged illustration highlights these seams in yellow. Each of these seams comprises a two-dimensional cubic diamond surface extending laterally relative to the layer. These seams represent lateral and vertical loop connection interfaces between adjacent layers. x The diamond-like joint in the network terminates on either side via a chiral pillar, as in Figure 36 The chiral columns (i.e., sp) are highlighted in red. 3 -sp 3 The chiral bars (keys) and chiral chains (highlighted in blue) are shown. Figure 37 In A, the data from... Figure 36 Two chiral pillars, in which, again, sp 3 -sp 3 The keys are highlighted in red, and the chiral chains are highlighted in blue. Figure 37 In B, the chiral column is illustrated, and... Figure 37 In C, the diagram illustrates the sp within the chiral column. x spiral.

[0486] Figure 36 The sp shown x The network represents a monomeric graphene system. The only atoms that are not monomers are the five primary carbon atoms in the z-space above the third layer. Since these atoms are not members of a ring, they cannot be members of a graphene structure or a graphene system.

[0487] exist Figures 29 to 36The modeled pyrolysis growth sequence connects all our observations in Study A. First, the non-uniform charging observed in the encapsulated bodies of sample A3 (see...) Figure 25 and Figure 27 This is attributed to sp at the geological tectonic interface. 3 Localization of grafting and diamond-like carbon (DLC) joints. These interfaces are most densely packed in the renucleation regions, which correspond to circular or near-defect areas on the template surface. On the other hand, regions with coating walls formed on flatter template surfaces exhibit less sp. 3 State and less charging. Secondly, because of sp across discontinuous geological interfaces. 2 and sp 3 Grafting eliminates many sp 2 Edge state, and because of sp 3 Grafting leads to activation throughout sp 2 Strong sp at the defect sites of the RBM phonons in the ring 2 -sp 3 Coupling, therefore sp 3 Grafting leads to sp 2 Intercalation of Raman D band. Finally, because the graft base is in sp 3 The grafted region contains elevated free radicals, so even if the template / substrate cannot be reached, higher layers can easily nucleate without inhibiting growth. This forms multilayer sp[s] constituting the ring-linked monomers. x Compared to the vdW assembly, the ring-connected unit exhibits superior mechanical robustness.

[0488] In Study A, we observed that the interpolation of the Raman D band increases with decreasing pyrolysis temperature. This is consistent with the slower hydrogen release at lower temperatures, allowing more time for the dynamic resorption condensates at tectonic interfaces to relax into energy-minimizing configurations. Therefore, eliminating high-energy sp at tectonic interfaces... 2 state sp 2 or sp 3 Grafting is promoted by lower temperatures.

[0489] In program A1, a CVD temperature of 750℃ achieves gradual dehydrogenation and carbonization of the condensate. This is beneficial for some sps at geological structural interfaces. 2 and sp 3 Grafting, and with sp 2 The condition was eliminated through grafting, and the D-band began to show potential interpolation patterns, such as its location at 1345 cm. -1 The average D above u The peak is located at 1343cm. -1 The average D at that location FThis is confirmed by the differences between the peaks. Based on this, we classify the encapsulated framework in sample A1 as a minimal grafting z-sp. x network.

[0490] In program A2, a CVD temperature of 1050 °C accelerates the dehydrogenation and carbonization of the condensate. High-energy edge dislocations are locked, resulting in vdW assemblages. RBM phonons are formed by these sp... 2 Since the edge state is activated, the D-band of sample A2 is not interpolated. Based on this, we classify the enveloped frame in sample A1 as a vdW assembly.

[0491] In procedure A3, the temperature is further reduced to 650°C to allow the grown condensate more time to rearrange and relax into sp. 2 The energy-minimizing graft configuration of the edge states. Therefore, sample A3 is located at 1340 cm. -1 D at the location u The peak reflects the highest D-band interpolation for any sample in study A and is located at approximately 1350 cm⁻¹. -1 sp at the place 2 Edge-activated D-band with 1332cm -1 Between the cubic diamond peaks. Based on this, we classify the enveloped framework in sample A3 as partially grafted z-sp. x network.

[0492] IX. Study B—Analysis

[0493] The samples generated and evaluated in Study B included coated frameworks synthesized on mesoporous or macroporous MgO templates via surface replication. Like samples A1 and A3, these samples exhibited excellent mechanical properties and included anthracite networks.

[0494] Figure 38 A is a SEM image of the coated composite material associated with procedure B1 before the extraction of the MgO template. Here, the content template can still be seen below the coating framework. The template consists of equiaxed particles with a porous substructure of co-nanocrystalline subunits formed through the thermal decomposition of the template precursor compound (magnesite or MgCO3). Figure 38 B is a SEM image of the encapsulated frames from sample B1, showing both the lack of removed templates and the preservation of the frames' native templated morphology. Figure 38 The appearance of the frame shown in B represents the appearance of the frames found in samples B2 and B3 made on similar template particles.

[0495] Figure 38C is a SEM image of the coated framework from sample B4. Sample B4 was synthesized by surface replication on a different template than samples B1–B3. This template comprises flat, plate-like particles with a porous substructure of joint nanocrystalline subunits derived from the thermal decomposition of a magnesite template precursor. Therefore, the coated frameworks in sample B4 exhibit a “cell-lamellae” morphology—similar to the frameworks in samples B1–B3 in terms of their porous substructure, but dissimilar in terms of their overall geometry.

[0496] In Study B, a lower pyrolysis temperature was explored to demonstrate the effect of a slower dehydrogenation rate in radical condensates, which theoretically could promote the condensates' ability to relax into energy-minimizing graft configurations at geological tectonic interfaces. Based on Study A, this is expected to produce fewer sp... 2 The edge states can be identified spectrally by the gradual interpolation of the D bands. The temperature of the CVD furnace was varied between 640°C and 540°C.

[0497] Table 4 below shows the sample, pyrolysis temperature (i.e., the set value on the CVD furnace), carbon source gas, and average. and Peak ratio, average G u and D u Peak position, and G u Peak and D u Inter-peak spacing:

[0498] Table 4

[0499]

[0500] * At 1318cm -1 With 1320cm -1 Repeated point spectra were found between

[0501] The average values ​​in Table 4 are derived from the average spectrum of a composite spectrum representing nine point spectra. To generate the average values, a moving average technique was first used at + / - 5 cm⁻¹. -1 The raw data from each point spectrum is smoothed within the wavenumber interval to minimize noise. After smoothing, the intensity values ​​from each point spectrum are normalized to a common scale, and then the normalized intensity values ​​are averaged to produce the average intensity value for each wavenumber.

[0502] Figure 39 A shows the average Raman spectra of samples B1 to B4. Figure 39 B shows the averaging of D. u Tr u and G u A magnified view of the features. Figure 39The black arrow in B indicates the direction of the corresponding spectral trend for programs B1-B3 as the CVD temperature decreases. Figure 39 C shows D u A magnified view of the peak, and Figure 39 D shows G u A magnified view of the peak.

[0503] Evaluation indicators D of the Raman spectra of samples B1-B3 u Peak intensity (and peak area) decrease with decreasing pyrolysis temperature. Peak FWHM appears to show no significant change. This trend of decreasing peak intensity and area is consistent with sp 2 The overall reduction in ring-associated RBM phonons. This is known in disordered carbon—in diamond-like carbon—sp 3 This occurs when the content increases, in the absence of sp. 2 In the case of a ring, the D feature completely disappears. Therefore, the reduced D observed in study B... u Peak intensity can be attributed to sp 2 The presence of the ring gradually decreases, and the ring is related to sp. 3 grafting-related sp 2 to sp 3 Rehybridization transforms into sp x As the pyrolysis temperature decreases, the condensate has more time to relax into low-energy spc particles at the geological interface. 3 The grafted configuration, and the increased ring disorder of the original domain, will sacrifice the horizontal region to promote the offset region. Both of these will increase sp 3 Grafting and sp x ring.

[0504] The evaluation of samples B1-B3 also showed that, in study B, as the CVD temperature decreased, D u The peak also gradually became dominated by low-frequency sp. 3 With more interpolation. This indicates sp 2 The prevalence of the decline in marginal states. As discussed in Study A, this indicates that at geological tectonic interfaces, an increasing number of sp... 2 The edges were eliminated, consistent with the use of a low-energy grafting configuration. Interestingly, the interpolation trend observed in samples B1-B3 did not extend to 1332 cm⁻¹. -1 Instead of stopping at the peak of the cubic diamond, it develops to even lower frequencies.

[0505] Surprisingly, as temperatures decreased and grafting was promoted, sp... 2The overall level of lattice distortion within the cluster also appears to be reduced. This is confirmed by the trend of higher valleys in samples B1–B3, a trend not observed in study A, where samples A1 and A3, although synthesized at lower temperatures than sample A2, exhibited higher valleys. This trend in study B could potentially be attributed to the influence of sp... 3 The increased prevalence of grafting, and especially by strain-strengthened sp... x The compression is explained by the increased prevalence of ring conformations (such as the boat conformation).

[0506] Another trend observed in samples B1-B3 is that, as the pyrolysis temperature decreases, G... u The peak position is at 1585cm -1 The usual position gradually shifted blue until it reached 1596.6cm. -1 This indicates that sp 2 -sp 2 The overall compressive strain of the bond increases, and this compression is also attributed to the increased grafting. Additionally, the G-band becomes narrower, indicating a smaller amplitude of strain state variation. Therefore, Study B confirms the correlation between grafting and compression observed in Study A. This compression also helps explain the decreased valley height. Figure 39 As can be seen from G u The increase in peak position, I Tru / I Gu The ratio decreases, indicating the tensile strain state as sp decreases. x The network is reduced due to greater compression.

[0507] Another spectroscopic observation in study B is that under 532 nm excitation, D... u The peak reached 1328.6cm. -1 (In sample B3) gradual interpolation below. Due to the 1328.6cm of sample B3. -1 D u Peak position and 1332cm -1 The cubic diamond peaks at these locations are close together, and since anthracite networks are known to be susceptible to beam-induced heating (which can affect D...), u (Peak position), therefore sample B4 was evaluated at a lower laser power setting of 0.5 mW. The Raman spectra collected for sample B4 at a 0.5 mW laser power setting ultimately confirmed that the D band redshifted to 1332 cm⁻¹. -1 Below the peak of the cubic diamond. At 1332nm. -1 The interpolation below indicates the hexagonal diamond arrangement in sp. x The existence of rings. Some researchers have demonstrated that hexagonal diamond at 1324.4 cm... -1 It exhibits a strong Raman peak at 1318 cm⁻¹, whereas in other cases it has been shown to be at 1318 cm⁻¹. -1With 1325cm -1 There are peaks between them. Therefore, the 1324.5 cm⁻¹ of sample B4... -1 Average D u Peak position, and D u Peak position is between 1318cm -1 With 1320cm -1 The multi-point spectrum between them is a non-chair conformation sp. x Strong evidence of rings.

[0508] In addition to a greater degree of interpolation, D in sample B4 u The band is also significantly narrower than D in samples B1-B3. u This indicates that a higher proportion of its RBM phonons are being generated by sp. x Backscattering at the interface is activated and is generated by the edge state sp. 2 The backscattered RBM phonons at these locations are being eliminated. 2 The more edge atoms are eliminated, and the more sp x The higher the grafting degree of the network, the narrower this peak becomes. This improvement in grafting in sample B4 can be attributed to three factors: (i) the strain required for grafting across certain geological structural interfaces. x The conformation is more stable at lower pyrolysis temperatures; (ii) the dehydrogenation rate is slower at lower pyrolysis temperatures, giving the condensate more time to seek graft configurations; and (iii) smaller C2H2 gas molecules with less steric hindrance are used.

[0509] We begin with the first factor, which is based on the premise that certain geological interfaces may not allow for chair conformation (i.e., cubic diamond). This premise aligns with previously published research on graphene-to-diamond bonding. In this work, we found that for the edge of a graphene domain to bond to the diamond surface, it is necessary for the atomic positions of the dangling graphene bonds to align with a specific sp atom present on the diamond surface. 3 The atomic positions of the atomic lines are matched as closely as possible. For certain graphene edge configurations, hexagonal carbon (i.e., hexagonal diamond) surfaces offer a more closely matched spline position compared to cubic diamond surfaces. 3 Atomic lines.

[0510] In our Figures 29 to 36 In the discussion, we explained that sp, including those with a chair-like configuration, x The diamond-like carbon (DLC) junction—that is, the cubic DLC junction. The graphene-diamond bonding from which the graphene edge configuration meets the splined surface of the diamond is required. 3 By extrapolating the existing technology of matching atomic lines, we reason that in order to achieve sp... 3Grafting: Each graphene edge must be grafted to a matching sp. 3 Atomic lines, and then these two sps 3 Atomic lines must be perfectly matched to form sp. 3 -sp 3 Bond lines. Sometimes this requires non-cubic polymorphs of diamond.

[0511] In which the edges are close enough to directly bond the hypothetical zigzag interface (such as... Figure 29 In the E1-E2 interface presented in the middle, two sp 3 Atomic wires can pass through the spline of the graphene edge itself. 2 to sp 3 Rehybridization (and then, because they are so close together, they can bond directly to each other) generates this. This effectively matches each of the two graphene structures to sp. 3 Atomic lines, and then sp lines are formed between them. 3 -sp 3 Bond lines are formed, thereby generating a two-dimensional cubic diamond-like joint.

[0512] However, since the spacing between edge atoms participating in geological structural interfaces is inherently random, we must consider that in some interfaces, opposing edge atoms may be too far apart to bond directly to each other. To illustrate this, in Figure 40 In image I, we involve two edges E * and E ** Modeling is performed on the offset zone of the zigzag-zigzag geological structural interface, where E ** Rise to E * Above. For simplicity, hydrogen atoms are not represented. Figure 40 The sp in screen I 2 The spacing between edge atoms is too large for sp to occur. 3 Grafting. However, space still exists between the edges for interstitial atoms to be inserted via continuous radical addition.

[0513] exist Figure 40 In scene II, we will sp 3 Interstitial atomic lines (in) Figure 40 (Circle out) Insert at the raised edge E ** This sp. 3 Interstitial atomic lines and E ** Edge matching and close enough to E * sp 2 Edge atoms are bonded, but vertical offset inhibits sp. 2 graft.

[0514] In scene III, E *The relative sp in 2 Edge atomic lines experience sp 2 to sp 3 Rehybridization, thus forming sp 3 Atomic lines, and these atoms are connected by sp. 3 -sp 3 Key (in) Figure 40 (Highlighted in red in image III) bonded to these interstitial atomic lines. This sp 3 -sp 3 Bonded loops connect the graphene structure. E ** The rise of the side sp 3 Free radicals allow for continuous radical addition, resulting in the formation of sp in a boat-shaped conformation. x Rings (because chair-like conformations are geometrically impermissible). As growth continues, seams can evolve, such as... Figure 40 As shown in image IV. This seam will no longer consist of cubic diamond, but rather of an amorphous hexagonal polymorph expected to have lower frequency Raman spectral peaks.

[0515] Therefore, the lateral spacing at the geological structural interface determines the distance through sp 3 sp of grafting evolution x The ring plays an important role in the configuration. If the spacing between the zigzag edges is close enough, it will be relatively sp 2 Edge atoms may be able to rehybridize and sp directly with each other. 3 Grafting, thus producing sp with a chair-like configuration. x Rings. If the spacing between the zigzag edges is too large, interstitial atomic lines can be inserted, and sp... 2 Edge atoms can be rehybridized, thus forming two sp atoms. 3 Atomic lines, these atoms can then form sp. 3 -sp 3 Bond lines. This will produce conformations with lower thermodynamic stability that may be unstable at higher temperatures, meaning that complete grafting of geological tectonic interfaces is impossible at higher temperatures. We can confidently conclude, based on the inevitability of these interface configurations and their influence on sp. exhibiting a boat-like conformation, that... x The need for a ring, if sp x The network is at 1332cm -1 The lower part did not show sp 3 If the D-peak of the pattern is interpolated, then it is an incomplete graft.

[0516] like Figure 40 The modeling in the paper shows that the insertion of interstitial atoms increases the local atomic filling density—in many interfaces, interstitial atoms can be filled or wedged into the interface, thereby compressing the sp around the interface. 2The fineness of this spacing, and the need for molecular rearrangement during dissociative adsorption, suggests that smaller gaseous substances (like C2H2) experience less steric hindrance due to reactions and insertion of atoms at these interfaces, thus promoting more grafting and compression. We suspect this is the primary reason why, although sample B4 (generated via C2H2 pyrolysis) was produced at the same temperature of 580 °C, it has a significantly lower D compared to sample 2 (generated via C3H6 pyrolysis). u Peak position.

[0517] The logic of atoms being tightly "filled" at geological structural interfaces applies not only to sp... 3 The offset region of grafting also applies to where sp occurs. 2 The horizontal region of the graft. The insertion of interstitial atoms at the geological structural interface explains the gradually increasing G peak position observed in study B, where sample B4 reaches 1603.3 cm⁻¹. -1 The average position and 1604.2cm -1 The point. In the process using C2H2 feed gas at pyrolysis temperatures below 580℃, we observed a value greater than 1606 cm⁻¹. -1 average G u Peak position, with a peak height of 1610cm. -1 .

[0518] It is easy to conceive of other randomly formed geological structural interfaces, and the sp at these interfaces 3 Grafting can evolve into other sps x Ring morphologies. These ring morphologies can include 5-membered rings, 7-membered rings, 9-membered rings, and possibly other rings, all of which are ring-connected and participate in the graphene structure. These sp... x Any sp of the ring 3 Grafting events can form diamond-like joints upon further processing.

[0519] As an example of this situation, in Figure 41 In image I, we show the geological interface formed by the zigzag edge segment and the armchair edge segment (i.e., the "zigzag-armchair" interface). For simplicity, we only show the offset region of the zigzag-armchair interface and again exclude hydrogen atoms. Figure 41 In screen I, the interface spacing makes the relative sp 2 Edge atoms are close enough to be directly grafted.

[0520] Therefore, sp 3 Grafting through these relative sp 2 sp of edge atoms 2 to sp 3 Rehybridization is performed, which forms two sp... 3Atomic lines, these atoms have the ability to form sps between two graphene structures. 3 -sp 3 The atomic positions of the bond lines. This is in Figure 41 As shown in screen II, sp 2 and sp 3 In the enlarged illustration, atoms are represented by solid black circles and black-and-white circles, respectively. 3 -sp 3 Bond lines form loops connecting alternating 5- and 7-membered splines of two graphene structures. x Ring (marked as R) a R b and R c And in Figure 41 (Highlighted in yellow in the enlarged illustration in Picture II).

[0521] like Figure 41 As shown in image III, the continuous pyrolysis growth from tertiary radicals can evolve into z-adjacent 5-membered and 7-membered rings (in... Figure 41 The Chinese standard is indicated by R. d R e and R f The second line and sp 3 The third line of the atom (indicated by black and white circles in the enlarged illustration of image III). Like the sp line adjacent to the z below it. 3 Atomic line, this sp 3 The atomic positions within the atomic lines can be incorporated into sp. 2 and sp 3 In the zigzag edges of the atoms, this is Figure 41 The enlarged illustration in image III circles this. In this way, a diamond-like joint is formed at the zigzag-armchair interface.

[0522] If the spacing of the zigzag-armchair interface is too large for bonds to form between opposing edge atoms, interstitial atoms may need to be inserted. In such cases, sp 3 Grafting can lead to boat-shaped and half-chair-shaped conformations—just as it does through interstitial atoms in zigzag interfaces. Figure 42 In image I, the edge atoms of the two domains are not close enough to directly graft onto each other, and the gap between them is sp. 3 The atoms have bonded to the edge of the armchair. This gap sp 3 Atomic lines are close enough to relative sp 2 Edge atoms form bonds, but vertical offset inhibits sp. 2 graft.

[0523] exist Figure 42 In scene II, sp 3 Grafting via sp2 sp of edge atoms 2 to sp 3 Rehybridization is performed, and the rehybridization cross-gap line forms a second sp. 3 Atomic lines, and sp lines are formed between the two lines. 3 -sp 3 Keyline. Sp 2 and sp 3 Atoms in Figure 42 In the enlarged illustration in image II, these are represented by solid black circles and black and white circles, respectively. 3 -sp 3 The bond forms a ring connecting the two domains with alternating 7-ary and 9-ary sp. x Ring (marked as R) I R II and R III And in Figure 42 (Highlighted in yellow in the enlarged illustration in Picture II).

[0524] like Figure 42 As shown in image III, continuous pyrolysis growth can evolve into a row of 6-membered rings (labeled R) with a boat-shaped conformation. IV R V and R VI (And highlighted in yellow in the enlarged illustration of image III). As shown in image IV, further growth can form a row of sps with a semi-chair-like configuration. x Ring (marked as R) VII R VIII and R IX And in Figure 42 (Marked in yellow in the enlarged illustration of image IV), thus generating Y dislocations. In this way, Y dislocations and hexagonal diamond-like joints are formed by interstitial atoms through a zigzag-armchair interface.

[0525] The random nature of the process inevitably leads to the existence of multiple geological structural interface configurations and sp. x While ring and diamond-like joints are discussed, the exemplary models detailed in this paper are sufficient to illustrate the dominant principles behind these diverse specific scenarios. They also explain the observed Raman spectral features consistent with cubic and hexagonal diamond phantoms.

[0526] Next, we consider more broadly the tectonic interactions and pyrolytic growth of a larger number of primordial domains, which generate higher-level tectonic activities that we have not yet considered. To illustrate this, we will use sp x The formation of the network is illustrated in the diagram. Figure 43 The diagram is drawn from a horizontal perspective. Growth is divided into three stages.

[0527] exist Figure 43In stage I, independently nucleated primordial domains grow toward each other on a common substrate. The substrate is colored blue, and black lines represent the growth domains. Arrows indicate that the primordial domains are growing radially outward based on radical addition at their edges. If growth stops during stage I, before significant grafting occurs, then sp 2 Radial breathing patterns will be primarily determined by sps associated with these isolated loop-disconnected regions. 2 Edge state activation.

[0528] exist Figure 43 In stage II, domain grafting forms a substrate and begins nucleation of higher layers on top of the substrate. This forms diamond-like joints (each joint in...). Figure 43 (represented by "X" in Phase II), and the anthracite sp associated with them. x Networks. Geological tectonic interfaces are inherently random and dynamic, where hydrogenated condensates rearrange and relax into energy-minimizing graft configurations. Some geological tectonic interfaces allow relatively edge atoms to graft directly onto each other, while others require the insertion of interstitial atoms (such as...). Figure 40 and Figure 42 (As shown) to achieve grafting. This increases atomic filling and in sp x This causes compression in the network. If growth terminates during stage II, the activation of RBM phonons will occur via sp 2 Edge state (remaining in place when growth ends) and sp 3 This occurs through a certain coordination of states. Therefore, we can expect some interpolation of the D-band, as well as different modes of the D-band.

[0529] exist Figure 43 In Phase III, sp x The steady state of vertical and lateral growth of the network drives the encounter and associated grafting of higher-level geological structures. Similar to the tectonic activity between primordial domains, this is stochastic. Dislocations tend to replicate z-periodically, thus generating lateral diamond-like joints, but this z-periodism is not deterministic. Simultaneously, new joints can nucleate through encounters with higher-level geological structures, as these encounters are also expected to produce discontinuous interfaces. This can contribute to the formation of dislocations throughout the sp... x A more even distribution within the network. If grown in Figure 43 If the phase III period is terminated, then the activation of the RBM phonon can be achieved by sp 3 The state is dominant (depending on the efficiency of grafting at the interface), and we can see more D-band interpolation compared to what we would see if growth were terminated during stage I or stage II.

[0530] Although we Figures 29 to 36The text describes vertical and lateral growth in stages, but anticipates lateral growth to be much faster than the vertical growth pattern. In other words, nucleation at higher levels may be rate-limiting. Since nucleation at higher levels occurs at tectonic interfaces, it could be accelerated by increasing tectonic activity and sp. 3 Grafting is used to accelerate overall growth. As long as the gas phase material is abundant, faster lateral growth achieves uniform substrate coverage and the formation of coating walls of consistent thickness. This explains our... Figure 27 The observation of uniformly thick coated walls in C—even in the “window” regions where nucleation in the original domain would be suppressed—has shown that on many substrates, the carbon produced remains linear over long periods, indicating a steady state of nucleation in higher layers. This “enduring” kinetic model is a fundamental advantage of anthracite networks over graphene networks, where the only growth mode is lateral growth.

[0531] G u Peak position (as a relative indicator of compressive strain), D u Peak position (as sp) 2 The relative indicators of the elimination of edge states) and therefore the spectral spacing between them (as compressive strain and sp) 2 The elimination of edge states (both metrics) can provide indicators for characterizing different sps. x A network has become a useful measure of the degree to which it forms graft bonds across various randomly formed geological interfaces during its growth. In this paper, it is defined as G. u Peak position and D u The interpeak spacing, the wavenumber distance between peaks, is commonly used in anthracite literature to determine vitrin reflectance via Raman spectroscopy. In turn, vitrin reflectance is a measure of coal maturity. As coal matures, its interpeak spacing widens, corresponding to an increase in vitrin reflectance. For immature to mature coals, using 532 nm excitation, previous researchers calculated vitrin reflectance as: vR0% = 0.0537(G u -D u )–11.21, where vR0% is the vitrinite reflectance (as calculated by Raman parameters).

[0532] In sample B4, the interpeak interval is 278.8 cm⁻¹. -1 This corresponds to a vitrinite reflectance of 3.76. This vitrinite reflectance is characteristic of anthracite. Beyond this value, the peak spacing is approximately 280 cm⁻¹. -1 The saturation point (slightly varying with excitation due to the dispersion of the D peak) causes the interval to begin to shrink again as anthracite matures into metamorphic anthracite and eventually into graphite. With this maturation process, The peak intensity ratio begins to increase, and the interpeak spacing is no longer useful for calculating vitrinite reflectance. For mature anthracite or metamorphic anthracite, 532 nm excitation is used, as previous researchers have used... Peak intensity ratio according to equation Calculate the reflectance of the vitrinite.

[0533] Next, we characterize sample B4 using XRD analysis. Figure 44 The overall XRD shape is shown. Table 5 below contains XRD peak angles, d-intervals, areas, area percentages (normalized to the area of ​​the main peak at 2θ = 24.489°), and full width at half maximum (FWHM) values ​​(uncorrected instrument broadening):

[0534] Table 5

[0535]

[0536] The XRD line shape of sample B4 includes broad peaks, indicating the extent of interlayer and in-plane periodicity. In particular, we note a broad fitted peak at 2θ = 43.138°, which is equivalent to... of <100> d-spacing. This reflects the graphite-based... of <100> The average in-plane compressive strain is approximately 2% of the spacing d. We can also see signs of in-plane compressive strain at 2θ = 79.501°, which is equivalent to... of <110> d-spacing. This again reflects the graphite-based... of <110> The compressive strain is approximately 2% of the d-spacing. This is consistent with the blue shift G exhibited by sample B4. u The peak positions are very consistent.

[0537] The most prominent feature of the XRD line shape of sample B4 is its main peak at 2θ = 24.489°, which reflects... of <002> d-spacing. This is significantly larger than that associated with AB-stacked graphite. <002> d-spacing or associated with mixed-layer graphite <002> d spacing. We attribute this expansion to the spread across sp. x Forced AA stacking at numerous cubic diamond-like carbon (CAD) seams in a network distribution. In the AA stacked regions, Pauli repulsion forces generated by the alignment of π electron orbitals are expected to increase the minimum interlayer spacing. Indeed, the interlayer spacing of AA stacked layers has been predicted to have… This is highly consistent with the interlayer main peak at 2θ = 18.454°. Additionally, we observed a related peak at 2θ = 50.192°. <004> Second peak, which reflects d-spacing — of <002> Half of the d-space.

[0538] The second interlayer peak fits at 2θ = 18.454°, which reflects... The interlayer spacing d. These values ​​and peak widths indicate a wide range of large interlayer spacings—larger than what we observed in study A. This is explained below. Due to the highly grafted x-sp x The increased atomic filling through grafting in the network induces in-plane compressive strain exceeding the critical buckling strain. Regions compressed beyond this critical buckling strain are forced to buckle in the positive z-direction, which represents their only degree of freedom. For this to occur, these regions need to overcome their vdW attraction to the underlying layer. This happens if they are sufficiently strained, and they bow out from the z-adjacent layer below, reaching a maximum z-deflection amplitude somewhere near the geometric center between the transverse seams anchoring their perimeter. This z-deflection alleviates the in-plane compressive strain in these regions but also increases their interlayer d-spacing. We expect the bowing to produce a broad continuum of interlayer d-spacing, which is precisely what we see in Table 4 and Figure 94 The broad peak observed, centered at 2θ = 18.454°, reflects a value greater than [missing information]. The interlayer spacing d is an important phase. Therefore, we attribute this second interlayer peak at 2θ = 18.454° to the z-direction bow-shaped bend of the xy compressed graphene regions between the diamond-like joints that pin them to the periphery.

[0539] Having established this association, we can even find the minimum grafting z-sp of sample A1. x We observed signs of arcuate bending in the interlayer spacing d of the network and sample A2 (vdW assembly), and we can also see that these samples also exhibit characteristics based on their <100> The in-plane compression of the peaks, these states indicate below The d-interval. Therefore, we can see that similar phenomena occur in these systems with fewer grafts. Specifically, in sample A2, it is very likely that a local sp... x Networks exist, but these networks do not extend throughout the entire envelope wall. In other words, the sp networks formed within the envelope wall of sample A2... x The network grafting is so poor that the ring-connected network cannot extend throughout the entire envelope wall.

[0540] Based on our findings in experiments A and B, it can be inferred in retrospect that sp may have already occurred in some graphite networks within the existing technology. 2 and sp 3 Examples of grafting.

[0541] In one such example, Cui employed a template-guided CVD procedure at 950 °C using methane (CH4) and MgO template particles, which produced a 1322 cm⁻¹ chromatogram on the template during synthesis.-1 D u The peak position (under 633 nm excitation) of a monolayer graphene structure. Excluding any interpolation of the D band, under 633 nm excitation, we would expect the peak D band of this graphene monolayer to be... u Appeared at 1332cm -1 Left and right. As we discussed, this will be related to sp. 3 Grafting and chair-shaped sp x The ring formation is consistent. Therefore, the reported 1322 cm -1 The reported D peak position can represent the redshift caused by interpolation.

[0542] However, we noticed a few points. First, regarding whether the program for Cui generates sp... 3 The grafting system satisfied us, and we attempted to replicate the reported results. We are pleased that the BET and TGA characterizations of the replicated sample we synthesized are in close agreement with the characterization of the sample reported by Cui. Furthermore, our Raman spectroscopy analysis (performed at 532 nm excitation) revealed... The Raman spectra were very similar in terms of peak intensity ratio. However, the analysis did not reveal any obvious interpolation at the D peak position. Our attempt to reproduce the interpolation of the D peak failed.

[0543] Secondly, regardless of the D-band interpolation in the samples reported by Cui, the samples cannot be described as anthracite networks or sp. x Because the generated graphene particles are natively monolayered when synthesized on the template, any crosslinking in the network is lateral. This is convincingly confirmed by extensive BET, TGA, and XRD characterization in the prior art. Therefore, the vertical crosslinking between layers provided by the anthracite network is not achieved, as these dislocations require a native multilayer structure. Indeed, monolayer networks have been reported to collapse into bilayer structures upon template removal. However, these bilayers do not crosslink via dislocations, thus sacrificing this important third dimension of molecular-level crosslinking present in the anthracite network. The lack of dislocations is evident in HRTEM images of bilayers, where the striations are uninterrupted, visually clear, and traceable at distances of 10 nm or greater.

[0544] In another prior art work, Chung synthesized carbon nanoonions in a flame at measurement temperatures of 700 °C or lower (the measurement temperature varied depending on the measurement location). This process involved rapid chemical vapor deposition on metal catalyst nanoparticles, thereby forming graphitic carbon nanoonions by precipitation. Based on our post-analysis, these graphitic carbon nanoonions appeared to include diamond-like carbon seams. However, considering the graphite arrangement of the layers constituting the hierarchical network (this graphite arrangement was evident in HRTEM analysis and also through the reported...), of <002> (The interlayer spacing was confirmed), and the crosslinking mechanism and pattern differ. In particular, these graphite networks exhibit far fewer chiral rings and chiral pillars due to a lack of transition zones at the geologically structured interfaces between their highly ring-ordered domains. These transitions are directly related to the wavy edge geometry associated with the ring-disordered domains grown via a radical cold polymer growth mechanism. Furthermore, these carbon nanoonions offer less versatility and reduced control over important morphological properties compared to the growth procedures presented herein. However, it is foreseeable that certain aspects of this flame synthesis process (such as partial oxidation) can be synergistically employed with the use of nonmetallic catalysts and radical cold polymer-based growth.

[0545] X. Research C—Analysis

[0546] In exploring ways to synthesize SP x In other pyrolysis procedures of the network, we found that template-guided CVD temperatures similar to those used in Study B but at lower temperatures (between 325°C and 500°C) produced increasingly brownish carbon. At 400°C and below, incomplete dehydrogenation of the condensate during growth produced carbon with a bright brown hue. At 460°C, the resulting carbon was gray with a slightly light brown tint.

[0547] A comparison of two samples (samples C1 and C2) synthesized at these temperatures. Figure 45 As shown in the figure. These color differences are similar to the differences between highly mature coal (black, low hydrogen) and less mature coal (brown, high hydrogen). Figure 45 The residual hydrogen in the 400°C carbon sample shown was confirmed by FTIR analysis, as... Figure 46 As shown.

[0548] Raman characterization of samples C1 and C2 was performed in an Ar atmosphere using a 532 nm laser with a power of 0.5 mW. This lower laser power was considered appropriate due to the thermal instability of the samples at higher powers. Table 6 below shows the sample, CVD temperature (i.e., the setpoint on the CVD furnace), carbon source, and average... and Peak intensity ratio, average G u and D u Peak position, and G u With D u Interval between peaks:

[0549] Table 6

[0550]

[0551] The Raman spectral data in Table 6 are derived from the average spectrum of a composite spectrum representing 16 points. To generate the average value, a moving average technique was first used at + / - 5 cm⁻¹. -1 The raw data from each point spectrum is smoothed within the specified interval. After smoothing, the intensity values ​​from each point spectrum are normalized to a common scale, and then the normalized intensity values ​​are averaged to produce the average intensity value for each wavenumber.

[0552] Compared to the samples in Study B, both samples C1 and C2 showed reduced interpeak spacing, consistent with more hydrogenation and less grafting. In sample C1, D u The peaks were interpolated, as shown in Table 6, and based on their position at 1332.7 cm⁻¹. -1 D at the location u Peak position, the particles in sample C1 constitute part of the grafted z-sp x Network. In sample C2, D u The peak did not show interpolation.

[0553] like Figure 47 The averaged spectra show that samples C1 and C2 are both at 600 cm⁻¹ -1 It exhibits a broad, weak peak at 600cm. -1 This peak has been attributed to dehydrogenated nanodiamond-type carbon and is also present in sample B4. Therefore, in addition to the hydrogenated phase associated with the decomposition products of uncarbonized free radical cold polymers in samples C1 and C2, there are indications of an unhydrogenated nanodiamond phase.

[0554] The coexistence of hydrogenated and dehydrogenated phases can correspond to phases grown inside and outside the porous template, respectively. That is, in addition to the increased stability of CH bonds at lower CVD temperatures inside the porous template (where gas exchange is diffusion-restricted), we also expect an increased proportion of H2. Unable to carbonize due to the inability to release molecular hydrogen, the radical condensates in such regions eventually relax back into neutral, lower molecular weight hydrocarbons. Workers in the field of radical condensates have demonstrated this phenomenon using time-of-flight mass spectrometry. To confirm this, a sample of C2 was immersed in ethanol under gentle stirring. This produced a stable amber dispersion that passed through a filter, indicating the dissolution of the oil phase of the hydrocarbon.

[0555] XI. Research D—Analysis

[0556] Study D was performed to confirm the role of H2 gas in inhibiting molecular hydrogen release during the growth of free radical accumulators. Procedures D1 and D2 were essentially the same, except that in procedure D1, only C3H6 and Ar were introduced into the reactor, while in procedure D2, a low flow rate of H2 was incorporated in addition to C3H6 and Ar. It was hypothesized that the presence of H2 would slow down the carbonization process and promote the relaxation of the cold polymer to an energy-minimizing graft configuration at the geological interface. Raman analysis was performed using a 532 nm laser with a power of 5 mW. Table 7 below shows sample ID, Raman D... u Peak position and approximate carbon yield in C@MgO coated composite powder:

[0557] Table 7

[0558]

[0559] D in sample D2 u Interpolation of the increased peak position confirmed the presence of increased H2, which facilitated the process D in sp. 2 Edge state elimination. Based on sample D1 at 1341.9 cm. -1 D u Peak position, the envelope framework in sample D1 includes partially grafted z-sp x Network. Based on sample D2, 1329.5cm -1 D u Peak position, the envelope framework in sample D2 includes highly grafted x-sp x network.

[0560] From the approximately 50% decrease in carbon growth, we can also see that the rate of carbon growth is slowed down by intensifying the carbonization of the cold polymer. Therefore, we find that H2 partial pressure can be used to suppress carbonization and improve grafting—especially at higher temperatures that accelerate carbonization. Based on this, we can infer that, in addition to pyrolysis temperature, the C:H ratio of the carbon source gas, the rate of H2 release and diffusion caused by growth, the presence of H2 feed gas, the morphology and pore structure of the substrate, the size of the template particles, the activity of the substrate surface, the presence of H2 scavenging substances, and many other factors are all important, as they all affect the dynamic equilibrium of hydrogenation and dehydrogenation in the radical cold polymer.

[0561] Understanding this allows for faster kinetics by rationally balancing these factors. As a simple example, we have observed that, compared to using a CVD temperature of 700°C and an H2 feed gas of 30 sccm, we can simultaneously achieve lower Di compared to using a CVD temperature of 580°C without H2 as the feed gas. u Peak position (and sp) 2 Better elimination of edge states (and faster carbon growth kinetics).

[0562] XII. Research E-analysis

[0563] Perform research E to demonstrate by sp x Network (referred to as "sp" in this article) x The precursor forms a helical x-network and z-network. Samples E1 and E2 are generated using the same template material and include sp x Precursors. Samples E1A and E2A are obtained by making samples E1 and E2 sp respectively. x It is formed through the maturation of the precursor. This maturation, or sp... 3 to sp 2 The rehybridization-induced transformation is achieved by altering the sp content before removing the MgO contents. x The precursor is annealed—that is, by annealing the C@MgO coated complex.

[0564] Equivalent quality samples E1 and E1A in Figure 48 The samples are shown side-by-side, with sample E1 on the left and sample E2 on the right. Sample E1 consists of large, hard particles, while sample E1A has a finer, softer consistency. The particles of sample E1 occupy a considerably smaller volume compared to the powder of sample E1A, and make a clicking sound against the glass wall of the vial when shaken, while the powder of sample E1A is silent when shaken. Sample E1A occupies a significantly larger volume.

[0565] Figure 49 A is a SEM image showing particles from sample E1. (Example) Figure 49 B and Figure 49 As shown at higher magnification, in sample E1, individual encapsulated bodies within macroscopic particles exhibit a cellular lamellar morphology similar to that of sample B4. The templates used to generate the samples in study E consisted of flat, plate-like particles, as well as stacks of plate-like particles. The template particles comprised porous substructures of combined nanocrystalline subunits derived from the thermal decomposition of the magnesite template precursor. These template particles (coated with iridium for imaging) are shown in the SEM images of Figure 51.

[0566] The flexibility of the coating walls in sample E1 and the surface tension of water during drying caused the collapse of intracellular pores, resulting in only lamellar superstructures (in Figure 49 (clearly shown in B) and fuzzy substructures (in Figure 49 The enlarged illustration in C clearly shows this. The localized flexibility of the coating wall in sample E1 gives the particles flexibility, such as... Figure 49As shown in B, this results in a wavy, tissue-like appearance. Visually tracing the edges of the lamellar particles in the SEM image reveals that no straight lines are easily found. The flexibility of the encapsulated framework in sample E1 allows the particles to conform to each other, thereby increasing their contact area and reducing the spacing between particles. It is the flexibility of the framework and the improved filling that forms dense, rigid particles during evaporation drying.

[0567] Figure 49 D is a SEM image showing the finer consistency of sample E1A powder compared to sample E1. Although agglomerates are still present in sample E1A, they are not as dense or rigid as the particles in sample E1, and many smaller agglomerates are present. The image shows the particle size distribution in sample E1A. Figure 49 E and the particles shown in sample E1 Figure 49 The comparison in B reveals a significant change. The particles in sample E1A appear straighter than the wavy particles in sample E1, indicating stiffening. The particles in sample E1 resemble paper towels, while the stiffened particles in sample E1A exhibit greater buckling angles. This increased stiffness reduces the ability of the particles in sample E1A to bend and conform to each other, thus hindering the degree of compaction exhibited by sample E1.

[0568] We can Figure 49 As seen in the magnified inset of F, the stiffening of the sample E1A particles is also evident at the local level, where the porous subunits retain their original morphology rather than collapsing. This makes... Figure 49 The porous substructure of sample E1A in F, which is clearly defined and identifiable, is obviously more porous than... Figure 49 The relatively ambiguous substructure of sample E1 in C is more faithful to the original templated morphology.

[0569] A similar comparison was made between samples E2 and E2A. Like sample E1, sample E2 densifies into rigid macroscopic particles, like... Figure 50 The particles shown in Figure A. At higher magnification, sample E2 particles can be seen within these particles. Like the particles of sample E1, the particles of sample E2 are wavy and flexible, as... Figure 50 B and Figure 50 As shown in C.

[0570] Compared to sample E2 powder, sample E2A occupies a significantly larger volume and has a finer uniformity. Compared to the larger, harder particles in sample E2, sample E2A powder consists of smaller, softer aggregates, such as... Figure 50 As shown in D. The annealed particles in sample E2A again exhibit a stiffening effect—both at the particle level and locally. The annealed particles in sample E2A are stiffer and straighter than the unannealed particles in sample E2, as shown in Figure D. Figure 50 E and Figure 50 As shown in F. Similarly, as Figure 50As shown in F, the plate-to-plate stacking observed in the template powder is retained in sample E2A powder, which may indicate that the plate-like particles fused together during annealing, preventing them from separating during the liquid phase extraction of the contents. The particle-to-particle fusion effect will be discussed further in conjunction with study F.

[0571] To understand the changes in the bonded structure resulting from annealing, Raman analysis was performed using a 532nm laser with a power of 5mW. Figure 52 G is shown u Peak and D u The average spectrum within the peak range, where spectral variations associated with annealing are indicated by black arrows. Table 8 below summarizes the average. and Peak intensity ratio, average G u Peak position and D u Peak position, and G u Peak position and D u Interval between peaks:

[0572] Table 8

[0573]

[0574] Interpolation D in samples E1 and E2 u Peak position indication associated with diamond-like carbon seam sp 3 The existence of the state. Based on sample E1 at 1335cm. -1 D u The peak position, the envelope framework from sample E1 includes partially grafted z-sp x Network. Based on sample E2, 1328cm -1 D u Peak position, the envelope framework from sample E2 includes highly grafted x-sp x Network. Their interpeak spacing is unique to anthracite.

[0575] In contrast, the mature samples E1A and E2A have D u The peak positions are 1352cm and 1352cm respectively. -1 and 1347cm -1 These peaks fall within sp. 2 The D band is within the normal range under 532 nm Raman excitation; therefore, maturation has eliminated sp in the coating framework of samples E1A and E2A. 2 Xianghe SP 3 Strong coupling of phases. This indicates that in samples E1A and E2A, the sp associated with the diamond-like joint is strong. 3 The state has been significantly reduced or eliminated. Their increase... Peak intensity ratio and reduced interpeak spacing reflect the maturity of the anthracite network. Based on sample E1A, D...u The peak position, whose framework includes highly mature helical z-carbons, and based on the D of sample E2A. u The peak position, whose framework includes highly mature helical x-carbons.

[0576] Considering the elimination of diamond-like carbon seams (which is for samples E1 and E2), x (The network provides a cross-linking mechanism), and surprisingly, the particles and coating walls in the mature sample become rigid. If these mature particles were not ring-connected, such thin-walled carbons would not survive template extraction, let alone with their sp... x The precursor is significantly harder. Therefore, we can conclude that the mature particles are cross-linked through a cross-linking structure that is harder than the atomically thin diamond-like seams of the precursor.

[0577] Besides their D u The peak returned to outside the normal D band range, and samples E1A and E2A also showed increased D. u and Tr u Peak intensity (relative to their G) u (peak), such as Figure 52 As shown in Figure D. u The increase in peak intensity (and area) reflects sp 2 The surge in rings. Along with the increase in sp. 2 Ring structuring, D u The deinterpolation of the peak confirms that sp x The ring transforms into p 2 ring sp 3 to sp 2 Rehybridization. The increased valley height of annealed samples indicates the relationship with sp. 2 The lattice distortion produces a consistent redshift mode of the G peak. 3 The elimination of the state, lattice distortion, and increased stiffness due to particle crosslinking together confirm the sp 3 to sp 2 Rehybridization is eliminating diamond-like carbon seams and forming sp 2 - Hybrid spiral dislocations. These spiral dislocations provide both vertical and lateral crosslinks and impose a helical geometry on the mature network. This helical network architecture can be conceptualized as a mesh formed by many loops of spiral dislocations, like... Figure 12 The grid shown in D.

[0578] To prove sp x The maturation of the precursor into a helical network was achieved through the study of sp... 3 to sp 2 Modeling the effect of rehybridization on diamond-like joints begins. Figure 53Image III shows a multi-layered monolith traversed vertically by cubic diamond seams. The system shown can be considered a much larger sp. x Small areas within the precursor system. Seams include sp. 2 -sp 3 Key and sp 3 -sp 3 The key—the latter is highlighted in red in screen I.

[0579] During annealing, such as Figure 53 As shown in screen II, the structure of sp 3 each member's sp 3 to sp 2 Rehybridization requires cleaving one of its bonds. This does not produce high-energy sp[s]. 2 In the case of free radicals, the two bonds cannot be broken. 3 -sp 3 Bonds are the most unstable and are the first to lose stability during annealing (these bond breaks in...). Figure 53 (Indicated by a gray dashed line). Because sp 3 Atoms and the sp between them 3 -sp 3 The bond line forms the lateral line, so one sp 3 Rehybridization of atoms, and their sp... 3 -sp 3 A cleavage of one of the bonds makes the xy adjacent sp along the bond line... 3 -sp 3 The bond becomes unstable, resulting in linear unlinking. The unlinking of the entire line produces a cleaved and sustained ABAB pattern—if sp 3 -sp 3 If a bond line breaks, the two adjacent z-bond lines are preserved to avoid the formation of high-energy sp-bond lines. 2 Free radicals.

[0580] In this way, through lateral unchaining, the diamond-like carbon seams are eliminated, and the associated loop connections between adjacent z-layers are also eliminated. Figure 53 The individual unit of image I therefore disintegrates into a distorted and broken vdW assembly. This is in Figure 53 As shown in Figure III. This clarifies the diamond-like carbon (DLC) joint in the transverse and vertical ring connections. x Its role in the network. During the disconnection, such as... Figure 53 As shown, the transverse crosslinking mode is retained, but the vertical crosslinking mode is eliminated. Based on this, we can conclude that sp x Network maturation eliminates the vertical crosslinking associated with diamond-like carbon (DLC) seams. If no other vertical crosslinking mechanism exists, maturation will... xThe precursor is transformed into a vdW assembly, and the rigidity of the vdW assembly without vertical crosslinking will be lower than that of its three-dimensional crosslinked precursor.

[0581] Next, we consider making sp with chiral rings and chiral pillars x The role of precursor maturation. Since we have already studied this system in A (see...) Figure 36 The formation model of ) is used, therefore we will use this model as an example sp x Precursors. However, to improve the visualization of their maturity, we only consider those from... Figure 36 Half of the system, said half from Figure 54 The two vertical and horizontal perspective views (H1 and H2) in picture I are shown. Similar to what we see... Figure 53 The precursor to modeling in the middle, Figure 54 The new precursor in image I includes a diamond-like joint. However, compared to... Figure 53 Unlike the precursor in the modeling, the diamond-like joint of the precursor terminates at a chiral pillar. The chiral pillar... Figure 54 The H2 perspective view of image I highlights the chiral chains, which are highlighted in blue, and connects the sp of adjacent chiral chains. 3 -sp 3 The keys are highlighted in red.

[0582] During the maturation period, sp 3 sp of the site 3 to sp 3 Rehybridization results in bond cleavage. 3 -sp 3 The sp bond is the least stable and the first to lose stability. The sp bond between the two terminal atoms of each chiral chain... 3 -sp 3 The key is broken. Each such key represents a horizontal sp. 3 -sp 3 The end of the bond line, and its cutting makes sp 3 -sp 3 The rest of the bond line becomes unstable. Therefore, sp 3 -sp 3 Linear unlinking of bond lines (previously in) Figure 53 (As shown in screen II) Figure 54 In scene II. These broken keys are... Figure 54 In image II, this is indicated by a gray dashed line. To avoid generating high-energy SP... 2 Free radicals, forming sp 3 -sp 3 ABAB pattern with key cut-off and retention.

[0583] exist Figure 54In the H1 perspective view of image II, we can see that, with these sp... 3 -sp 3 The unlinking of bonds eliminates the diamond-like carbon (DLC) seams in the system. Upon their elimination, the associated vertical crosslinks also disappear, while the transverse crosslinks remain. Without chiral rings or chiral pillars, this loss of vertical crosslinks would again result in a broken z-adjacent layer VdW assembly, just as it does in... Figure 53 As shown in the system. However, in this case, chiral columns exist, and ABAB cleavage causes sp within the chiral columns to... x The bonds in the helix remain intact. This occurs because the sp bonds between the terminal atoms of each chiral chain remain intact. 3 -sp 3 When the bond breaks, the z-adjacent sps between chiral rings 3 -sp 3 The bonds are preserved, thus maintaining consistency with the broken and preserved ABAB pattern. These preserved bonds are due to sp 3 to sp 2 Rehybridization and transformation into sp 2 -sp 2 Key. This will be a one-dimensional sp x The spiral transforms into a form including sp 2 Atoms and sp 2 -sp 2 One-dimensional sp of the key 2 Spirals. These bonds are in... Figure 54 The H2 perspective view in image II is highlighted in blue. Although the vertical crosslinks associated with the diamond-like carbon seam are lost, this sp... (The sentence is incomplete and requires further context to translate accurately.) 2 The retention of the helix ensures that the system retains the vertical crosslinks associated with the chiral columns. Therefore, both lateral and vertical crosslinks are preserved during maturation. The chiral rings (and the associated chiral columns connecting the chiral rings) are key to preserving the vertical crosslinks during maturation.

[0584] This retention of transverse and longitudinal crosslinks Figure 54 As shown in image III, this diagram represents the relaxed system shown in image II. From image III, we can see that the helical ribbon-like graphene structure formed through maturation has a z-oriented helical dislocation at its center. (Central sp) 2 The atoms in the helix are in a ring at sp 3 to sp 2 All members before and after rehybridization. Therefore, during maturation, sp 2 The formation of the spiral is accompanied by sp 2 The spiral as an edge segment belongs to the adjacent sp 2 The formation of the helical path of the ring. Therefore, from sp 2From the formation of the spiral, we can deduce sp 2 The formation of graphene helices, to which helices belong, and from which they are formed by sp 2 The retention of vertical crosslinking of the helix allows us to infer the retention of vertical loop connectivity.

[0585] We can see from Figure 54 As seen in image III, the helical graphene structure must be twisted to preserve vertical ring connectivity. The graphene helical dislocations have been shown to exhibit torsional strain, and along with this torsional strain, we expect to see a surge in lower-frequency strain-induced phonon states. The higher troughs in samples S1A and S2A demonstrate this lattice distortion caused by this helical geometry. Furthermore, we can see from... Figure 54 In scene III, we see sp 3 The state is swapped to sp 2 Edge state. sp 3 State elimination and sp 2 The surge in edge states is caused by D in samples E1A and E2A u Peak position deinterpolation reflection. (Compared to sp) x ring to sp 2 ring-related sp 2 The surge in rings was observed in samples E1A and E2A with an increase in D. u This is reflected in the peak intensity. Therefore, the formation of helices around the chiral column explains several spectral variations associated with maturation.

[0586] Including sp 2 The edge segments of the helical pattern represent an interesting structure. While it includes a zigzag edge configuration, its uniqueness lies in the fact that each atomic member of the segment is bonded to three nearest-neighbor carbon atoms, whereas in a normal zigzag edge configuration, only half of the edge atoms are bonded to three carbon atoms. This unique property of the helical zigzag pattern stems from the fact that it represents an atomic chain generated by a broken polygon, where the interior angles of the broken polygon are all less than 180°, thus allowing for three carbon neighbors at each edge site (as opposed to a normal zigzag edge, which includes an anti-angle that prevents each edge site from bonding to three carbon atoms). This novel edge configuration can produce novel electromagnetic and thermal properties known to depend on the edge configuration in graphene nanoribbons.

[0587] To further clarify the role of sp x Spiral evolution into sp 2 In the spiral process, we are Figure 55 The transformation is illustrated in the diagram. Figure 55 In screen I, a chiral column with three adjacent z-shaped chiral rings is shown. Figure 55 The blue lines in the diagram represent bonds in a chiral chain, while the red lines represent sp... 3 -sp3 key. Figure 55 The black circle in the middle represents sp 2 Atoms, and black and white circles represent sp. 3 atom.

[0588] During maturation, sp within each chiral ring 3 -sp 3 The bond breaks, just as we previously bound. Figure 54 As discussed in Scene II, this leads to the production of sp 3 -sp 3 The ABAB pattern with key breakage and retention. The sp_sp_ indicating the breakage of the "B" phase in the ABAB pattern. 3 -sp 3 Key in Figure 55 In screen II, this is represented by a gray dashed line and marked "B". Simultaneously, the reserved sp of phase "A" in the ABAB mode is also indicated. 3 -sp 3 The bond is transformed into sp through rehybridization. 2 -sp 2 Keys. Correspondingly, these keys are in Figure 55 In screen II, this is represented by a blue line and marked "A". The result is obtained through sp 2 -sp 2 key-connected sp 2 A one-dimensional helical chain of atoms. During relaxation, this sp... 2 The curvature of the spiral becomes more uniform, such as Figure 55 As shown in screen III.

[0589] Next, we consider the transformation of two-dimensional graphene structures around these one-dimensional helices. As we have established, sp 2 The formation of a helix is ​​necessarily accompanied by the formation of graphene helices, within which sp 2 Spirals represent edge segments. Figure 56 The diagram in the middle reflects Figure 55 The difference lies in the diagram. Figure 56 In the middle, we try to represent around sp x Spiral and sp 2 The spiral's ring-connected structure allows us to graphically illustrate the formation of its helical geometry. Figure 56 In screen I, we show the ending where we... Figure 55 The diagram in image I illustrates the diamond-like joints of the same chiral pillars (extending into the foreground, as indicated by the translucent portion of the diagram). The chiral chains within these rings... Figure 56 In screen I, it is again represented by a blue line, and sp 3 -sp 3The key is again indicated by a red line. To maintain consistency with our established conventions, Figure 56 The black circle in image I represents sp 2 Atoms, and black and white circles represent sp. 3 Atoms. However, in Figure 56 In this diagram, we use solid blue and red regions to represent loop connection spaces. For example, the blue space surrounding a blue chiral chain represents the loop connection sp around the chiral chain. 2 Space. The red space indicates the ring connection sp associated with the diamond-like carbon joint. 3 space.

[0590] During the ripening period, Figure 56 The center sp in picture I x Spiral experience we are Figure 55 The same transformation is illustrated in the diagram. That is, the sp within each chiral ring. 3 -sp 3 The key is broken, and thereafter, as Figure 56 As shown in image II, the related sp 3 -sp 3 Keyline unlinking. This eliminates the loop connection sp associated with the "B" in the ABAB pattern. 3 The spatial portion. In Figure 56 In image II, we represent this eliminated space as gray and label it "B," which we can imagine extending into the foreground of the diagram, much like the diamond-like joint shown in image I. Meanwhile, the retained sp of the "A" phase, representing the ABAB mode, is also represented. 3 -sp 3 Bond lines are transformed into sp lines through rehybridization. 2 -sp 2 Keyline. The reserved loop connection space of this "A" phase is in... Figure 56 In image II, it is represented in blue and marked "A". We can also imagine it extending into the foreground of the diagram, like the diamond-like seam shown in image I.

[0591] Upon relaxation, a single helical graphene structure is produced, such as... Figure 56 As shown in screen II, where... Figure 55 The same one-dimensional sp of the picture III 2 The helix (e.g., a screw dislocation) is located at its center. The parametric equations approximating this helix are x = u cos(v), y = u sin(v), z = cv, where the value of u is greater than or equal to sp from the center. x One-dimensional sp of spiral evolution 2 The radius of the spiral.

[0592] These diagrams illustrate sp with diamond-like joints and chiral rings.x How network maturation can generate mature networks with lateral and vertical loop connections. To illustrate the principle of this transformation, we utilize a network comprising a single diamond-like carbon seam and a single sp... X Spiral sp x Precursor. However, a considerable amount of sp x The network may consist of numerous joints and chiral loops formed through interactions and grafting between geological structures. In many cases, such as in our... Figure 36 As shown, the encounter of a single geological structure between two edge segments can evolve into multiple joints and chiral rings.

[0593] For this reason, it is expected that a simple exemplary sp including multiple seams and chiral rings will be provided. x The transformation of the precursor is modeled. Since we have already studied this system in research A (see...) Figure 36 We model the formation of ), and for this current purpose, we return to it. We do this by... Figures 29 to 36 The geological structures shown in the figure meet and subsequently undergo pyrolysis growth, leading to this hypothesis. x Network. To facilitate a visual assessment of the system's transformation, we start from... Figure 57 The system is shown in two vertical and horizontal perspective views (H1 and H2).

[0594] exist Figure 57 In screen I, we can see that sp x The precursor includes two distinct diamond-like carbon seams (each seam is circled in the H2 perspective view), and chiral posts representing the lateral ends of these seams (in the H2 perspective view, the chiral chains are highlighted in blue, and the sps connecting the chiral chains are also shown). 3 -sp 3 (Keys are highlighted in red). During the maturation period, sp 3 to sp 2 Rehybridization results in sp within each chiral ring 3 -sp 3 Bond breaking, such as bonding Figure 54 The system in (which is itself) Figure 57 The transformations of the subsystems of the system considered in the discussion, such as those that can be reviewed, are addressed here. Figure 57 As shown in screen II, where gray dashed lines are again used to represent broken sp. 3 -sp 3 Key. sp 3 -sp 3 The ABAB pattern of keyline cutting and retention is based on the already combined Figure 54 The system transformation discussion proceeds sequentially. The retained keys are transformed into sp... 2 -sp 2 Key (in) Figure 57(Highlighted in blue in the H2 perspective view of screen II). Figure 54 and Figure 57 The only significant difference between the transformations shown is that Figure 57 The transformation across a larger span x Multiple seams and chiral ring extensions of the precursor.

[0595] Figure 57 The relaxation of the system shown in screen II Figure 57 The spiral network shown in Figure III. This unit comprises a network of two combined spiral regions formed by two different helical dislocations of the system. The spiral regions are interconnected in loops, although... Figure 57 The horizontal perspective view in the image is not ideal fo...

Claims

1. A synthetic anthracite, said synthetic anthracite comprising a coated framework, said framework comprising a templated graphene network crosslinked via Y-dislocations, said synthetic anthracite having at least one of a mesoporous structure and a macroporous structure, and characterized by an average Raman spectrum at 532 nm, said average Raman spectrum including values ​​between 1300 cm⁻¹ and 1300 cm⁻¹. -1 With 1332 cm -1 The unfitted D peak between.

2. A synthetic anthracite, said synthetic anthracite comprising a coated framework, said framework comprising templated helical x-carbon crosslinked via helical dislocations, said synthetic anthracite having at least one of a mesoporous structure and a macroporous structure, and characterized by an average Raman spectrum at 532 nm, said average Raman spectrum including values ​​between 1342 cm⁻¹ and 1442 cm⁻¹. -1 With 1375 cm -1 The unfitted D peak between.

3. The synthetic anthracite as described in any one of claims 1 to 2, wherein the synthetic anthracite comprises an environmental superconductor.

4. The synthetic anthracite as described in any one of claims 1 to 2, wherein the synthetic anthracite is macroscopic.

5. The synthetic anthracite as described in any one of claims 1 to 2, wherein the synthetic anthracite comprises a collapsed cell structure.

6. The synthetic anthracite as described in claim 1, wherein the synthetic anthracite comprises sp x network.

7. The synthetic anthracite as described in claim 2, wherein the synthetic anthracite is formed by maturing the synthetic anthracite as described in claim 1.

8. The synthetic anthracite as claimed in claim 1, wherein the synthetic anthracite is further cross-linked through mixed dislocations.

9. The synthetic anthracite of claim 8, wherein the mixed dislocations comprise chiral pillars.

10. The synthetic anthracite of claim 2, wherein a portion of the spiral dislocation comprises a double spiral dislocation.

11. The synthetic anthracite as claimed in claim 1, wherein the synthetic anthracite comprises sp 2 Hybrid regions and diamond-like regions.

12. The synthetic anthracite of claim 11, wherein the diamond-like region comprises at least one of cubic diamond, hexagonal diamond, and amorphous diamond.

13. The synthetic anthracite of claim 11, wherein the diamond-like region comprises at least one of the following: chair conformation, boat conformation, and semi-chair conformation.

14. The synthetic anthracite of claim 11, wherein the diamond-like region comprises having sp 2 Hybrid atoms and sp 3 sp of both hybrid atoms x ring.

15. The synthetic anthracite as claimed in any one of claims 1 to 2, wherein the synthetic anthracite comprises ring-linked monomers.

16. The synthetic anthracite according to any one of claims 1 to 2, wherein the synthetic anthracite comprises a content of less than 2,300 m³ as measured by N₂ adsorption. 2 Minimum average BET surface area per g.

17. The synthetic anthracite as claimed in any one of claims 1 to 2, wherein the synthetic anthracite comprises an N2 adsorption density between 1,000 m³ and 1,000 m³. 2 / g and 2,300 m 2 Minimum average BET surface area between / g.

18. The synthetic anthracite as claimed in any one of claims 1 to 2, wherein the synthetic anthracite comprises an amount of N2 adsorption measured at 10 m... 2 / g and 1,000 m 2 Minimum average BET surface area between / g.

19. The synthetic anthracite according to any one of claims 1 to 2, wherein the synthetic anthracite comprises an atom with a density of less than 10.0 cm⁻¹ as measured by N₂ adsorption. 3 / g average BJH specific porosity.

20. The synthetic anthracite of claim 19, wherein the synthetic anthracite comprises an N2 adsorption density between 7.5 cm⁻¹ and 1.5 cm⁻¹. 3 / g and 10.0 cm 3 The average BJH porosity between / g.

21. The synthetic anthracite of claim 19, wherein the synthetic anthracite comprises an N2 adsorption density between 2.5 cm⁻¹ and 2.5 cm⁻¹. 3 / g and 7.5 cm 3 The average BJH porosity between / g.

22. The synthetic anthracite as described in claim 1, wherein the unfitted D peak is between 1318 cm⁻¹. -1 With 1332 cm -1 between.

23. The synthetic anthracite as described in claim 1, wherein the unfitted D peak is between 1300 cm⁻¹. -1 With 1318 cm -1 between.

24. The synthetic anthracite as described in any one of claims 1 to 2, wherein the average Raman spectrum at 532 nm includes a range between 1580 cm⁻¹ and 1580 cm⁻¹. -1 With 1595 cm -1 The unfitted G peaks between.

25. The synthetic anthracite as described in any one of claims 1 to 2, wherein the average Raman spectrum at 532 nm includes a range between 1595 cm⁻¹ and 1595 cm⁻¹. -1 With 1610 cm -1 The unfitted G peaks between.

26. The synthetic anthracite as described in any one of claims 1 to 2, wherein the average Raman spectrum at 532 nm includes those with a value higher than 1610 cm⁻¹. -1 The unfitted G peak.

27. The synthetic anthracite according to any one of claims 1 to 2, wherein the average Raman spectrum at 532 nm includes a range between 600 nm and 600 nm. -1 With 750 cm -1 The unfitted peaks between.

28. The synthetic anthracite as claimed in any one of claims 1 to 2, wherein the average Raman spectrum at 532 nm includes a valley between the unfitted G peak and the unfitted D peak, wherein the ratio of the height of the valley to the height of the unfitted G peak is between 0.60 and 0.

80.

29. The synthetic anthracite as claimed in any one of claims 1 to 2, wherein the average Raman spectrum at 532 nm includes a valley between the unfitted G peak and the unfitted D peak, wherein the ratio of the height of the valley to the height of the unfitted G peak is between 0.40 and 0.

60.

30. The synthetic anthracite as claimed in any one of claims 1 to 2, wherein the average Raman spectrum at 532 nm includes a valley between the unfitted G peak and the unfitted D peak, wherein the ratio of the height of the valley to the height of the unfitted G peak is between 0.20 and 0.

40.

31. The synthetic anthracite as claimed in any one of claims 1 to 2, wherein the average Raman spectrum at 532 nm includes a valley between the unfitted G peak and the unfitted D peak, wherein the ratio of the height of the valley to the height of the unfitted G peak is between 0.05 and 0.

20.

32. The synthetic anthracite as described in any one of claims 1 to 2, wherein the average Raman spectrum at 532 nm includes an I value less than 3.0 between its unfitted D peak and unfitted G peak. D / I G Peak intensity ratio.

33. The synthetic anthracite as described in claim 32, wherein the average Raman spectrum at 532 nm includes an I value between its unfitted D peak and unfitted G peak, which is between 2.0 and 3.

0. D / I G Peak intensity ratio.

34. The synthetic anthracite as described in claim 32, wherein the average Raman spectrum at 532 nm includes an I value between its unfitted D peak and unfitted G peak, which is between 1.0 and 2.

0. D / I G Peak intensity ratio.

35. The synthetic anthracite as described in claim 32, wherein the average Raman spectrum at 532 nm includes an I value between its unfitted D peak and unfitted G peak, which is between 0.1 and 1.

0. D / I G Peak intensity ratio.

36. The synthetic anthracite as described in any one of claims 1 to 2, wherein the average Raman spectrum at 532 nm includes an I0.50 between its unfitted 2D peak and unfitted G peak. 2D / I G Peak intensity ratio.

37. The synthetic anthracite as described in any one of claims 1 to 2, wherein the average Raman spectrum at 532 nm includes an I value between its unfitted 2D peak and unfitted G peak, which is between 0.25 and 0.

50. 2D / I G Peak intensity ratio.

38. The synthetic anthracite as described in any one of claims 1 to 2, wherein the average Raman spectrum at 532 nm includes an I value between 0.05 and 0.25, representing the unfitted 2D peak and the unfitted G peak. 2D / I G Peak intensity ratio.

39. The synthetic anthracite as claimed in any one of claims 1 to 2, wherein the XRD profile of the synthetic anthracite includes an unfitted profile corresponding to an average interlayer spacing d of 3.35 Å to 3.45 Å. <002> Peak position.

40. The synthetic anthracite as claimed in any one of claims 1 to 2, wherein the XRD profile of the synthetic anthracite includes an unfitted interlayer spacing d corresponding to an average interlayer spacing between 3.45 Å and 3.55 Å. <002> Peak position.

41. The synthetic anthracite of claim 1, wherein the XRD profile of the synthetic anthracite includes an unfitted interlayer spacing d corresponding to an average interlayer spacing between 3.55 Å and 3.65 Å. <002> Peak position.

42. The synthetic anthracite of claim 1, wherein the XRD profile of the synthetic anthracite includes an unfitted interlayer spacing (d) corresponding to an average interlayer spacing (d) between 3.65 Å and 4.00 Å. <002> Peak position.

43. The synthetic anthracite of claim 1, wherein the XRD shape of the synthetic anthracite includes peaks corresponding to an extended interlayer spacing d greater than 3.75 Å. <002> Component peaks.

44. The synthetic anthracite of claim 1, wherein the XRD profile of the synthetic anthracite includes peaks corresponding to an extended interlayer spacing d between 3.75 Å and 4.50 Å. <002> Component peaks.

45. The synthetic anthracite of claim 1, wherein the XRD profile of the synthetic anthracite includes peaks corresponding to an extended interlayer spacing d between 4.50 Å and 5.25 Å. <002> Component peaks.

46. ​​The synthetic anthracite of claim 1, wherein the XRD profile of the synthetic anthracite includes peaks corresponding to an extended interlayer spacing d between 5.25 Å and 6.00 Å. <002> Component peaks.

47. The synthetic anthracite as claimed in any one of claims 1 to 2, wherein the XRD shape of the synthetic anthracite includes unfitted peaks corresponding to an average intralayer spacing of less than 2.13 Å. <100> peak.

48. The synthetic anthracite as claimed in any one of claims 1 to 2, wherein the XRD profile of the synthetic anthracite includes unfitted peaks corresponding to an average intra-layer spacing d between 2.11 Å and 2.13 Å. <100> peak.

49. The synthetic anthracite of claim 1, wherein the XRD profile of the synthetic anthracite includes unfitted peaks corresponding to an average intra-layer spacing d between 2.09 Å and 2.11 Å. <100> peak.

50. The synthetic anthracite of claim 1, wherein the XRD shape of the synthetic anthracite includes unfitted peaks corresponding to an average intra-layer spacing d between 2.00 Å and 2.09 Å. <100> peak.

51. The synthetic anthracite according to any one of claims 1 to 2, wherein the coating framework comprises microparticles, the microparticles comprising at least one of the following: spherical particles, fibrous particles, rose-shaped particles, cubic particles, prism-shaped particles.

52. The synthetic anthracite as claimed in claim 2, wherein the synthetic anthracite is a macroscopic body comprising at least one of the following: grains, flakes, fabrics, paper, filaments, and molded articles.

53. The synthetic anthracite as claimed in claim 3, wherein the environmental superconductor comprises environmental superconducting grains, and the graphene network comprises particulate environmental superconductivity.

54. The synthetic anthracite of claim 3, wherein the environmental superconductor comprises a porous material evacuated to an internal pressure of less than 760 Torr.

55. The synthetic anthracite as claimed in claim 53, wherein the environmental superconductor is evacuated to an internal pressure between 1 Torr and 10 Torr.

56. The synthetic anthracite as claimed in claim 53, wherein the environmental superconductor is evacuated to an internal pressure between 100 millitor and 1 torr.

57. The synthetic anthracite as described in claim 53, wherein the environmental superconductor is evacuated to internal pressures of 10 mTorr and 100 mTorr.

58. The synthetic anthracite of claim 53, wherein the environmental superconductor is evacuated to an internal pressure below 10 millitor.

59. The synthetic anthracite as described in claim 3, wherein the environmental superconductor comprises a gas-impermeable barrier phase.

60. The synthetic anthracite as described in claim 59, wherein the gas impermeable barrier phase comprises a metal.

61. The synthetic anthracite of claim 3, wherein the environmental superconductor comprises a macroscopic product, the macroscopic product comprising a continuous filament, a sheet, or a molded component.

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