Using a composition of matter in an induction melting furnace

Abstract

Innovative techniques for forming unique material compositions and the various advantageous physical properties and associated properties of the resulting materials are revealed. Specifically, metals (including various alloys, such as ingot nickel superalloys) are characterized by the presence of carbon within their metallic lattice structure. This carbon is primarily or entirely present at interstitial sites within the metallic lattice and can be present in amounts ranging from about 15 wt% to about 90 wt%. Furthermore, this carbon forms nonpolar covalent bonds with the metal atoms of the lattice and other carbon atoms present in the lattice. This contributes to the substantially uniform dispersion of carbon within the resulting material, thereby providing unique and advantageous properties such as strength-to-weight ratio, density, mechanical toughness, shear strength, flexural strength, hardness, corrosion resistance, electrical conductivity, and / or thermal conductivity, as described herein. In some methods, the material composition can be pulverized or the powder can be granulated.

Description

Technical Field

[0001] This disclosure generally relates to the manufacture and use of carbon-containing alloys in induction melting furnaces. Prior Technology

[0002] Specialty alloys are smelted in vacuum induction melting (VIM) furnaces. The crucible of such VIM furnaces is used to melt and mix various mixtures of components (e.g., metals and nonmetals). Once the various combinations of metals are mixed, the melt can be poured (e.g., into) a mold and cooled. Some mixtures include powdered components. Unfortunately, the electromotive force from the induction coil of the VIM furnace acts on the powder, causing it to be ejected from the VIM furnace. This prevents the powder from mixing with other components. An improved method is needed for using powdered components in vacuum induction melting furnaces.

[0003] As used herein, the term "covetic material" refers to a metal containing carbon particles of nanometer size. Covetic materials are desirable in a variety of applications because they possess many physical, chemical, and electrical properties that surpass those of conventional non-carbon-containing materials. Summary of the Invention

[0004] The present invention is provided to introduce, in a simplified form, a series of concepts further described below in the detailed embodiments. The present invention is not intended to identify key or essential features of the claimed subject matter, nor is it intended to limit the scope of the claimed subject matter. Furthermore, the systems, methods, and apparatuses disclosed herein each have several inventive forms, and each of these inventive forms is not solely responsible for the attributes disclosed herein.

[0005] The various embodiments of the subject matter disclosed herein generally relate to apparatus, methods, and various compositions of carbon-metal composite materials. The apparatus shown and discussed may relate to the controlled use of plasma spraying torch equipment to produce various carbon-metal bonded material compositions, which are generally referred to in this disclosure as "covetic materials." In some cases, these materials are metal-decorated carbon. In some cases, these materials are carbon-decorated metal. In other cases, as described in more detail below, carbon may be combined with materials other than metals (such as ceramics, plastics, composite materials, silicon, etc.).

[0006] One configuration of a plasma spraying torch comprises a reaction chamber, a microwave energy source, and a controller. The reaction chamber is configured to contain a hydrocarbon process gas mixed with a plurality of molten metal nanoparticles. The microwave energy source is operatively coupled to the reaction chamber to provide power. The controller is used to adjust the microwave energy source to create conditions within the reaction chamber such that the hydrocarbon process gas dissociates into its constituent carbon atoms, and monolayer graphene (SLG) or few-layer graphene (FLG) grows from these carbon atoms onto the molten metal nanoparticles to form a plurality of carbon-metal nanoparticles. In some configurations, the conditions within the reaction chamber cause: (i) a first temperature at which carbon atoms dissolve into the molten metal nanoparticles; and (ii) a second temperature at which at least some of the dissolved carbon atoms combine with the molten metal in a certain crystal configuration. Some configurations of the device utilize cooling zones to cool the plurality of carbon-metal nano-sized particles into powder form, which can be collected and stored in a storage container located adjacent to and alongside the reaction chamber.

[0007] According to various embodiments, the inventive concept disclosed herein can be embodied in a composition of substances having any of the following physical and / or structural properties and associated properties. Furthermore, according to different embodiments, these properties and / or properties may be included in different combinations or arrangements, but are not limited thereto.

[0008] In one embodiment, a material composition comprises one or more particles, each particle independently comprising a metal lattice having one or more coherent planar graphene layers disposed therein. Preferably, at least some carbon atoms of the one or more coherent planar graphene layers are disposed in interstitial sites within the metal lattice. More preferably, the one or more coherent planar graphene layers are interspersed between the basal planes of the lattice. Graphene may exist as a single layer (e.g., "single-layer graphene" or "SLG") or multiple layers (e.g., two layers, three layers, five layers, ten layers, or any number of layers up to fifteen, also referred to herein as "few-layer graphene" or "FLG"). At least some carbon atoms of the one or more graphene layers are covalently bonded to metal atoms of the metal lattice, and the covalent bonds between the carbon atoms and the metal atoms are nonpolar covalent bonds or include nonpolar covalent bonds. In some embodiments, the covalent bonds may consist substantially or entirely of nonpolar covalent bonds. Similarly, carbon atoms of the one or more graphene layers may be covalently bonded to other carbon atoms of the one or more graphene layers, and depending on the implementation, these covalent bonds may include nonpolar covalent bonds, consist substantially of nonpolar covalent bonds, or consist entirely of nonpolar covalent bonds. Therefore, the one or more particles may substantially or completely lack polar covalent bonds. Likewise, the metal lattice of each particle may substantially or completely lack ionic bonds. The one or more graphene layers are preferably substantially defect-free, making the graphene "pristine". Preferably, each particle is also characterized by substantially lacking or more preferably completely lacking carbon aggregates and / or agglomerates at grain boundaries and / or at the surface of the metal lattice. Due to the innovative processing technology described herein, the total carbon loading of the particles can range from about 15 wt% to about 90 wt%, and various intermediate loadings are also demonstrated (e.g., in various embodiments, about 20 wt%, about 25 wt%, about 33 wt%, about 40 wt%, about 50 wt%, about 60 wt%, about 75 wt%, or up to 90 wt%). Furthermore, these particles are characterized by a diameter in the range of about 20 nm to about 3.5 μm, and / or having a maximum distinguishable feature size in the range of about 0.1 nm to about 1 µm. In some embodiments, these particles can be compressed into pellets.

[0009] According to another embodiment, a material composition comprises an indium nickel alloy having carbon disposed within its crystal lattice. Preferably, at least some of the carbon atoms are disposed at interstitial sites of the metal lattice, and more preferably, the carbon is substantially uniformly dispersed within the metal lattice. Furthermore, in some embodiments, the grain boundaries and / or surfaces of the material composition are substantially free of carbon aggregates and / or agglomerates. Therefore, the maximum identifiable feature size of the material composition can be in the range of about 0.1 nm to about 1 µm. At least some carbon atoms are covalently bonded to metal atoms of the metal lattice, and the covalent bonds between the carbon atoms and the metal atoms are nonpolar covalent bonds or include nonpolar covalent bonds. In some embodiments, these covalent bonds may consist substantially of or entirely of nonpolar covalent bonds. Similarly, carbon atoms may be covalently bonded to other carbon atoms, and according to different embodiments, these covalent bonds may include nonpolar covalent bonds, consist substantially of nonpolar covalent bonds, or consist entirely of nonpolar covalent bonds. Therefore, the composition of one or more substances may substantially or completely lack polar covalent bonds. Similarly, a metal lattice may substantially or completely lack ionic bonds.

[0010] According to another embodiment, a material composition comprises a metal lattice in which at least about 15 wt% carbon is disposed. Preferably, at least some of the carbon is disposed at interstitial sites of the metal lattice, and more preferably, the carbon is substantially uniformly dispersed in the metal lattice. Furthermore, in some embodiments, the grain boundaries and / or surfaces of the material composition are substantially free of carbon aggregates and / or agglomerates. Therefore, the maximum identifiable feature size of the material composition can be in the range of about 0.1 nm to about 1 µm. At least some carbon atoms are covalently bonded to metal atoms of the metal lattice, and the covalent bonds between the carbon atoms and the metal atoms are nonpolar covalent bonds or include nonpolar covalent bonds. In some embodiments, such covalent bonds may consist substantially or entirely of nonpolar covalent bonds. Similarly, depending on the implementation, carbon atoms can be covalently bonded to other carbon atoms, and these covalent bonds can include nonpolar covalent bonds, consist substantially of nonpolar covalent bonds, or consist entirely of nonpolar covalent bonds. Therefore, the composition of one or more substances may substantially or completely exclude polar covalent bonds. Likewise, a metal lattice may substantially or completely exclude ionic bonds.

[0011] In various embodiments of the foregoing embodiments, the metal lattice may include one or more metals selected from the group consisting of: aluminum, copper, iron, nickel, titanium, tantalum, tungsten, chromium, molybdenum, cobalt, manganese, niobium, and combinations thereof. Therefore, the metal lattice may be characterized by a crystal structure such as face-centered cubic (FCC), body-centered cubic (BCC), or hexagonal close-packed (HCC). Furthermore, the metal lattice may contain approximately 15 wt% to approximately 90 wt% carbon (e.g., in various embodiments, approximately 20 wt%, approximately 25 wt%, approximately 33 wt%, approximately 40 wt%, approximately 50 wt%, approximately 60 wt%, approximately 75 wt%, or up to 90 wt%). Carbon is preferably present at interstitial sites within the metal lattice. In some methods, the metal may be present in alloy form. For example, in a particularly preferred method, the metal may be in the form of one or more Inconel alloys, such as Inconel 600, Inconel 617, Inconel 625, Inconel 690, Inconel 718 and / or Inconel X-750. More preferably, the Inconel alloy is a superalloy.

[0012] The following description, in conjunction with the accompanying drawings and specification, elaborates on one or more embodiments of the subject matter described in this disclosure. Other features, aspects, and advantages will become apparent from this specification, the accompanying drawings, and the claims. It should be noted that the relative dimensions in the following figures may not be drawn to scale. Simple Explanation of the Diagram

[0013] The embodiments of the subject matter disclosed herein are shown by way of example and are not intended to be limited to the figures in the accompanying drawings. Throughout the drawings and description, similar element symbols denote similar elements. It should be noted that the relative dimensions in the following figures may not be drawn to scale. Figure 1A is a comparative diagram illustrating two different covetic material forming techniques according to some embodiments, and exemplary materials produced by applying each of these covetic material forming techniques. Figure 1B presents high-resolution transmission electron microscopy and high-resolution energy dispersive X-ray images of materials (e.g., covetic materials) produced according to the innovative technology described herein according to some embodiments. Figure 2 illustrates a manufacturing process for growing graphene onto small molten particles according to one or more of the disclosed embodiments. Figure 3 depicts a plasma energy state diagram according to one or more of the disclosed embodiments, illustrating how a pulsed microwave energy source can be used to grow graphene onto small molten particles. Figure 4 illustrates an electronic temperature control technique for growing graphene onto small molten particles according to one or more of the disclosed embodiments. Figure 5 illustrates a dual plasma torch apparatus for growing graphene onto small molten particles according to one or more of the disclosed embodiments. Figure 6 illustrates a pulsed microwave plasma spraying torch apparatus adapted for growing graphene onto small molten particles according to one or more of the disclosed embodiments. Figure 7 is a diagram depicting the intersection of common subject areas associated with covetic (or related materials), plasma torch spraying, and / or robust synthetic composite carbon coatings according to one or more of the disclosed embodiments. Figures 8A-B are schematic diagrams depicting a plasma spraying process for spraying carbon particles onto small molten particles according to one or more of the disclosed embodiments. Figure 9 is a scanning electron microscope image showing the effect of spraying carbon particles onto small molten particles according to one or more of the disclosed embodiments. Figure 10 shows a graph depicting the graphene growth temperature profile and a binary phase diagram according to one or more of the disclosed embodiments. Figure 11 is a cross-sectional view of a conventional plasma flame device. Figure 12 illustrates a pulsed microwave process flow used in growing graphene onto small molten particles according to one or more of the disclosed embodiments. Figure 13 is a perspective view of a conventional pulsed microwave plasma spraying waveguide device used to grow graphene onto small molten particles. Figure 14 is a schematic depiction of a micro-welding technique for growing graphene onto small molten particles according to one or more of the disclosed embodiments. Figure 15 is a schematic depiction of a plasma spraying apparatus in a coaxial configuration according to one or more of the disclosed embodiments. Figure 16 is a schematic depiction of a plasma spraying apparatus according to one or more of the disclosed embodiments, illustrating the evolution of a material processed under a series of non-equilibrium energy conditions. Figure 17 illustrates a surface wave plasma system for growing graphene onto molten particles according to one or more of the disclosed embodiments. Figures 18A1-2, 18B, 18C and 18D depict various configurations of plasma spraying reactors according to one or more of the disclosed embodiments. Figure 19 is a graph depicting energy versus time during pulse turn-on and pulse turn-off according to one or more of the disclosed embodiments. Figure 20A1 is an image depicting the organometallic bonding that occurs when carbon and copper are combined using a plasma spraying torch, according to some of the embodiments disclosed. Figure 20A2 is an image depicting a graded material composition applied to a substrate material according to some of the disclosed embodiments, showing multiple (such as three) material property regions. Figure 20B is a material evolution diagram depicting several layered configurations that occur when carbon is added to the bulk aluminum, according to one or more of the disclosed embodiments. Figure 21A depicts an apparatus according to one embodiment for spraying a molten mixture of materials onto a substrate. Figure 21B depicts a method for spraying material (e.g., covetic material) onto a substrate according to one or more of the disclosed embodiments. Figure 21C is a schematic diagram depicting a plasma spraying process for spraying a film according to one or more of the disclosed embodiments. Figure 22A depicts an apparatus for encapsulating carbon particles with a molten material (e.g., metal) according to one or more of the disclosed embodiments. Figure 22B depicts a method for encapsulating carbon particles with a molten material (e.g., metal) according to one or more of the disclosed embodiments. Figures 23A, 23B, 23C and 23D depict exemplary deposition techniques according to one or more of the disclosed embodiments. Figures 24A and 24B depict simplified schematic diagrams of materials according to one or more of the disclosed embodiments, which are formed by conventional deposition techniques for placing such materials onto a substrate. Figures 25A and 25B depict simplified schematic diagrams of materials formed by an innovative deposition technique that produces nonpolar covalent bonds on a substrate surface using one or more of the disclosed embodiments. Figures 26A, 26B, 26C, 26D, and 26E depict schematic diagrams illustrating how nonpolar covalent bonds can be formed between sites in the square shape of the face-centered cubic (FCC) structure of aluminum and sites in the hexagonal shape that appear in certain crystal structures of carbon. Figure 27A depicts an exemplary apparatus for producing a material (e.g., a covetic material) in powder form, according to one or more of the disclosed embodiments. Figures 27B1 and 27B2 depict exemplary fluidized bed apparatus for cooling and processing powdered materials (e.g., powdered covetic) in a fluid, according to one or more of the disclosed embodiments. Figure 27C is a schematic diagram depicting a plasma spraying process for producing powdered materials (e.g., powdered covetic materials) according to one or more of the disclosed embodiments. Figure 28 illustrates a method for manufacturing components from powdered materials (e.g., powdered covetic materials) using injection molding technology according to some embodiments. Figure 29 illustrates various properties of the materials (including covetic materials) described herein according to various embodiments. Figures 30A1 and 30A2 depict problems and solutions associated with molten powder (e.g., metallic decorative carbon) compared to the same or similar materials molten in pellet form, according to some embodiments. Figure 31 illustrates a method, according to some embodiments, of using pellets to minimize or remove material ejection during the introduction of pellets into a VIM furnace. Figure 32 depicts melt placed in a mold according to some embodiments. Figure 33 illustrates a simplified schematic diagram of a puck processing technique and equipment based on a given pattern. Figure 34 shows a simplified schematic diagram of a disc dispersion test process according to one method. Implementation

[0014] Related applications

[0015] This patent application is an international application claiming priority to the following: U.S. Patent Application No. 17 / 957,937, filed September 30, 2022, entitled “USING PELLETIZED METAL-DECORATED MATERIALS IN AN INDUCTION MELTING FURNACE” (subsequently published on May 11, 2023, under the same title as U.S. Patent Publication No. 2023-0145800); and U.S. Patent Application No. 17 / 957,989, filed September 30, 2022, entitled “USING PELLETIZED METAL-DECORATED MATERIALS IN AN INDUCTION MELTING FURNACE” (subsequently published on February 9, 2023, under the same title as U.S. Patent Publication No. 2023-0040722). All disclosures of prior applications are considered part of this patent application and are incorporated herein by reference.

[0016] This disclosure relates to methods for producing covetic materials using spraying techniques rather than by mixing carbon-based materials into a molten metal slurry. Some embodiments relate to techniques for reducing the size of interstitial carbon structures to the nanometer (nm) scale. The accompanying figures and discussion present exemplary environments, systems, and methods for producing "covetic" materials, which are generally understood and defined herein as implying a high concentration (>6% wt and up to 90% wt) of carbon integrated into other materials (such as metals, metal-containing materials, plastics, composites, ceramics, etc., according to various embodiments as described herein) in a manner that prevents carbon separation during melting or magnetron sputtering. The resulting materials possess many unique and modified properties compared to the base materials from which they are produced. Carbon is dispersed in the matrix (e.g., metallic) in several ways that contribute to improving material properties. For example, carbon is very strongly bonded to the resulting material (e.g., covetic materials), often resisting many standard methods in detecting and characterizing its form. The inclusion of nanoscale carbon increases the melting point and surface tension of the resulting material. Materials produced according to the techniques described herein exhibit higher hot and cold working strength. [, Identification and Importance of Problems and Opportunities , ] [, , ]

[0017] Metal matrix composites can be composed of a matrix of (at least) a metal or metal alloy (referring to a metal made by combining two or more metallic elements (especially to provide higher strength or corrosion resistance)) combined with high-strength modulus ceramics, carbon-based reinforcements, or microfillers in the form of continuous or discontinuous fibers, whiskers, or particles. The size of the reinforcement is important because micron-sized reinforcing metals can exhibit higher strength and stiffness than the base alloy, up to acceptable levels. However, such improvements can also be accompanied by undesirable poor ductility and undesirable low yield strength, machinability, and fracture toughness under critical loads due to undesirable, non-uniform carbon placement between particles during processing (e.g., at grain boundaries). To avoid premature cracking and other drawbacks in metal matrix composites with incompatible micron-sized reinforcements, reducing the size of the reinforcing phase to the nanoscale is crucial. In addition, various methods are needed to incorporate the reinforcing phase into the matrix (e.g., a metal alloy), and ideally, to incorporate the reinforcing phase uniformly into the matrix.

[0018] Corresponding to the addition of the aforementioned carbon-based reinforcements, significant improvements in mechanical, thermal, electrical, and tribological properties have been observed. Notably, these properties may be altered and / or improved when the size of the reinforcement is reduced from the micrometer scale (e.g., 1-1000 µm) to the nanometer scale (e.g., <100 nm) due to increased cohesion between the matrix and particles. This improvement in properties can be attributed to the formation of strong interfaces that promote efficient reinforcement mechanisms. It has been reported that nano-sized particles (~20 nm) exhibit enhanced tensile and yield strength compared to micrometer-sized particles (~3.5 μm), although the volumetric loading of nano-sized particles is reduced by an order of magnitude. Therefore, prior art techniques known in the art, such as induction melting and plasma spark sintering, typically cannot provide nanometer-sized reinforcements. Thus, there is a current need to reduce the carbon structure containing interstitial vacancies to the nanometer scale. [, microwave , ] [, (MW) , ] [, Plasma torch reactor , ] [, , ]

[0019] Using a microwave (MW) plasma torch reactor, pristine 3D few-layer graphene (FLG) particles can be continuously nucleated, such as during flight in atmospheric pressure vapor streams of carbonaceous materials like methane gas, where such nucleation occurs in the initially synthesized carbon-based or carbon-containing "seed" particles. Highly structured and tunable 3D mesoporous carbon-based particles, consisting of multiple layers of FLG (e.g., 5-15 layers), grow from the carbonaceous material, accompanied by the incorporation of metallic elements or metal-based alloys, to form at least partially covalently bonded (and at least partially metallically bonded or ionicly bonded) carbon-metal composite (also referred to herein as "covetic") particle structures. In some embodiments, the "pristine" graphene (referring to defect-free or very defect-free graphene) provided or produced in the described MW torch reactor is unoxidized or contains extremely low (e.g., < 1%) oxygen content. In some embodiments, the metals (in the resulting covetic material) are held together by metallic bonding, and the carbons (common in graphene or other organized carbon-based 2D or 3D structures such as a matrix or lattice) are held together primarily by nonpolar covalent bonds. Composite carbon-metal structures may include nonpolar covalent bonds between carbon atoms and metal atoms present at the metal-carbon interface. In a preferred embodiment, the covalent bonds between carbon atoms and / or between carbon atoms and metal atoms in the material composition consist substantially or entirely of nonpolar covalent bonds.

[0020] Furthermore, carbon can be present in amounts unattainable by conventional techniques. For example, according to various embodiments, the resulting material may contain greater than about 6 wt% carbon, greater than about 15 wt% carbon, greater than about 40 wt% carbon, greater than about 60 wt% carbon, or up to about 90 wt% carbon. In various embodiments, carbon may be contained in the aforementioned amounts within the metal lattice such that all or substantially all of the carbon is incorporated into the metal (or other material) lattice, and there are substantially or no carbon aggregates and / or agglomerates at the grain boundaries / lattice surfaces. Furthermore, carbon is preferably located at interstitial sites within the lattice.

[0021] In a particularly preferred embodiment, the material may be provided in the form of a powder having the physical properties of a "covetic" material as described herein. The powder may comprise a plurality of particles, for example, particles with a diameter of about 20 nm to about 3.5 µm, each particle comprising metallic decorative carbon (in the form of carbon-on-metal or metal-on-carbon) having carbon disposed in a metal lattice as described herein. Preferably, each particle independently comprises a metal lattice, the metal spacer having one or more (e.g., one, two, five, ten, or up to fifteen) coherent planar graphene layers disposed within the metal lattice. Figures 21C and 27C show an exemplary cross-sectional structure of such coherent planar graphene layers disposed along the basal surface of an aluminum substrate, according to one aspect of the inventive concept currently described. Those skilled in the art will appreciate that various embodiments of the powder currently described may include particles exhibiting such a cross-sectional structure. Indeed, because the carbon is incorporated into the lattice, the carbon advantageously diffuses into the basal surface rather than precipitating at grain boundaries (or other lattice surfaces). This process is possible because of the wettable nature of nanoscale graphene, and it is not observed when producing carbon implant materials using conventional techniques.

[0022] In various embodiments, at least some carbon atoms of one or more coherent planar graphene layers are disposed in interstitial sites within a metal lattice, and preferably, one or more coherent planar graphene layers are juxtaposed parallel to the basal plane of the metal lattice. In some embodiments, one or more coherent planar graphene layers are interspersed between the basal planes of the metal lattice. In some embodiments, one or more coherent planar graphene layers are interspersed between the basal planes of the metal lattice. Those skilled in the art will understand upon reading this disclosure that this unique dispersion of carbon at the interstitial sites and its arrangement relative to the basal plane of the lattice occurs due to the innovative processing described herein, which utilizes the high "wetability" of nanoscale graphene (particularly virgin graphene) and, as described herein, achieves high carbon loading, substantially uniform carbon dispersion, and substantially lack of carbon aggregates and / or agglomerates, all of which are not achievable using conventional techniques. See, for example, Figures 1A-1B, for a graphical comparison of conventionally produced "covetic materials" and materials produced using the innovative technology described herein, as well as the corresponding descriptions below.

[0023] Continuing with reference to the powdered material according to this disclosure, at least some of the carbon atoms can be covalently bonded to metal atoms in a metal lattice, while also allowing nonpolar covalent bonding between carbon atoms and / or metallic bonding between metal atoms of the material. More specifically, the nonpolar covalent bonding between carbon atoms and / or between carbon atoms and metal atoms is characterized by the equal sharing of electrons among the bonded atoms, which differs from polar covalent bonding (where electrons are shared among the bonded atoms) or ionic bonding (where the bonded atoms remain together due to charge differences after electrons are transferred from one atom to another). In some states, the particles of the powdered material may substantially or completely exclude polar covalent bonds and / or ionic bonds. In this context, "substantially" excluding polar covalent bonds and / or ionic bonds means a composition whose properties (e.g., crystal structure, mechanical strength, thermal / electrical conductivity, reflectivity, etc., as described below, and in particular, see Figure 29) are not due to the presence of polar covalent bonds and / or ionic bonds. Compositions that substantially do not contain polar covalent bonds and / or ionic bonds can be considered to consist essentially or entirely of nonpolar covalent bonds, at least in terms of the carbon and metal atoms bonded together within the structure.

[0024] Furthermore, graphene is preferably "pristine" because its 2D or 3D structure is essentially free of defects such as vacancies, inclusions, contaminants, etc., as those familiar with this technology will understand after reading this disclosure.

[0025] The metallic lattice may include one or more metals, such as aluminum, copper, iron, nickel, titanium, tantalum, tungsten, chromium, molybdenum, cobalt, manganese, niobium, and combinations thereof. Where combinations are included, the metals are preferably in alloy form, such as Inconel superalloys, preferably Inconel superalloys formed from nickel, chromium, aluminum, copper, iron, titanium, tantalum, molybdenum, cobalt, manganese, and / or niobium, and most preferably, Inconel superalloys are Inconel 600, Inconel 617, Inconel 625, Inconel 690, Inconel 718, Inconel X-750, or combinations thereof. In some cases, the combination includes tin and / or tungsten, and / or silver, and / or antimony, individually or in combination. In some embodiments, one or more of the aforementioned metals may be used individually or in combination as a surfactant to improve the wettability of the metal-carbon combination.

[0026] Powdered materials, as described herein, are preferably formed using non-equilibrium plasma, such as those produced using microwave plasma-based reactors as described herein. The currently disclosed microwave plasma-based reactor process provides a reaction and processing environment in which gas-solid reactions can be controlled under non-equilibrium conditions (referring to a physical system that is not in thermodynamic equilibrium but can be described by variables, which are extrapolations used to specify variables for a system in thermodynamic equilibrium; non-equilibrium thermodynamics involves transport processes and chemical reaction rates, as well as the initial melting of the metal powder, which can be independently controlled by ionization potential and momentum, and thermal energy).

[0027] Following in-situ nucleation (meaning in-situ within a reactor or reaction chamber), solid, basic solid, or semi-solid carbon-based particles detaching from the plasma torch can be additively deposited layer-by-layer onto a temperature-controlled substrate (such as a roller). The detached particles can be sprayed onto and bonded to a specific substrate. In some cases, no substrate is used; instead, groups of detached semi-solid particles form one or more oriented, independent, self-supporting structures. Unlike standard plasma torches with limited operating flow rates, power, and configuration, currently disclosed microwave plasma torches incorporate control mechanisms (such as flow control, power control, and temperature control) to independently control the temperature and gas-solid reaction chemistry of one or more constituent materials to produce unique, etched, highly structured, covalently bonded carbon-metal structures with surprisingly high homogeneity.

[0028] For illustrative purposes, according to various embodiments, the maximum distinguishable feature size of a uniformly dispersed metal-carbon assembly (e.g., defined by the length measured along the longitudinal axis of the "feature") is in the range of about 0.01 nanometers (nm) to 1 micrometer (µm), preferably in the range of about 0.01 nm to about 1 µm, more preferably in the range of about 0.01 nm to about 750 nm, more preferably in the range of about 0.01 nm to about 500 nm, more preferably in the range of about 0.01 nm to about 100 nm, and in some range, more preferably in the range of about 0.01 nm to about 50 nm, and most preferably in the range of feature sizes of about 0.01 nm to about 10 nm. This is in contrast to non-uniform dispersion, which is characterized by a relatively large feature size of about a few (e.g., 3-5) micrometers or larger.

[0029] The composition may also include a plurality of "aggregates" and / or a plurality of "fossils," wherein each aggregate comprises a large number of particles linked together, and each floc comprises a large number of aggregates linked together. In some embodiments, each particle may have a principal size between 20 nm and 150 nm. Each aggregate may have a principal size between 40 nm and 10 µm. Each floc may have a principal size between 0.1 µm and 1,000 µm.

[0030] Covetic materials produced by currently revealed MW reactor-based technologies offer a variety of competitive advantages not previously available in current materials or products. One such advantage involves inherent scalability and versatility for formulation of unique, physically and chemically stable, multifunctional metal-carbon composites exhibiting predictable deformation (in terms of stress, strain, elasticity, or some other determinable physical property) in various configurations and / or architectures such as (but not limited to): (1) dense film implantation; (2) coating; (3) thick strips; and (4) powdered particles capable of withstanding subsequent remelting and casting and / or forming engineered metal alloy components. Compared to existing parent metal alloy formulations, any of the aforementioned dense film MW reactor-produced carbon-based metal composite implants and / or coatings and / or strips and / or powdered particles exhibit enhanced physical, chemical, and electrical properties.

[0031] Materials produced using powders (and / or pellets formed from such powders) as described above enjoy many of the same advantageous physical properties and characteristics as powders themselves, except that micron-sized materials may not exhibit the presence of carbon in coherent planar layers disposed along the basal planes of a metal lattice. Rather, micron-sized materials (e.g., produced by microwave plasma spraying torches or other suitable techniques described herein (and equivalents that a person skilled in the art will understand upon reading such descriptions)) are characterized by carbon loadings (e.g., from 1.5 wt% to 90 wt%, and any amount therein) that have not been achieved to date, uniform / uniform dispersion of carbon in a metal matrix, and the absence of carbon aggregates and / or agglomerates at lattice surfaces (e.g., grain boundaries). Apart from this distinction, the final products produced using powdered materials (preferably powdered covetic materials) can exhibit any one or more physical properties and / or characteristics (in any combination) of the powdered precursors without departing from the scope of the inventive concept described herein. [General Implementation]

[0032] According to a general example, a material composition comprises one or more particles, wherein each particle independently comprises a metal lattice having one or more coherent planar graphene layers disposed therein.

[0033] According to another general example, a material composition comprises an indium nickel alloy having carbon disposed in the lattice of the indium nickel alloy.

[0034] According to another general example, a material composition comprises a metal lattice having at least about 15 wt% carbon disposed therein.

[0035] Furthermore, in various embodiments, the aforementioned state may include any of the following physical and / or structural characteristics and associated properties. Moreover, according to different embodiments, these characteristics and / or properties may be included in different combinations or arrangements, but are not limited thereto.

[0036] In one embodiment, a material composition comprises one or more particles, each particle independently comprising a metal lattice having one or more coherent planar graphene layers disposed therein. Preferably, at least some carbon atoms of the one or more coherent planar graphene layers are disposed in interstitial sites within the metal lattice. More preferably, the one or more coherent planar graphene layers are interspersed intermittently between the basal planes of the metal lattice. Graphene may exist as a single layer (e.g., "single-layer graphene" or "SLG") or multiple layers (e.g., two layers, three layers, five layers, ten layers, or any number of layers up to fifteen, also referred to herein as "few-layer graphene" or "FLG"). At least some carbon atoms of the one or more graphene layers are covalently bonded to metal atoms of the metal lattice, and the covalent bonds between the carbon atoms and the metal atoms are nonpolar covalent bonds or include nonpolar covalent bonds. In some embodiments, the covalent bonds may consist substantially or entirely of nonpolar covalent bonds. Similarly, carbon atoms of the one or more graphene layers may be covalently bonded to other carbon atoms of the one or more graphene layers, and depending on the implementation, these covalent bonds may include nonpolar covalent bonds, consist substantially of nonpolar covalent bonds, or consist entirely of nonpolar covalent bonds. Therefore, the one or more particles may substantially or completely lack polar covalent bonds. Likewise, the metal lattice of each particle may substantially or completely lack ionic bonds. The one or more graphene layers are preferably substantially defect-free, making the graphene "pristine". Preferably, each particle is also characterized by substantially lacking or more preferably completely lacking carbon aggregates and / or agglomerates at grain boundaries and / or at the surface of the metal lattice. Due to the innovative processing technology described herein, the total carbon loading of the particles can range from about 15 wt% to about 90 wt%, and various intermediate loadings are also observed (e.g., in various embodiments, about 20 wt%, about 25 wt%, about 33 wt%, about 40 wt%, about 50 wt%, about 60 wt%, about 75 wt%, or up to 90 wt%). Furthermore, these particles are characterized by a diameter in the range of about 20 nm to about 3.5 μm, and / or having a maximum distinguishable feature size in the range of about 0.1 nm to about 1 µm. In some embodiments, these particles can be compressed into pellets.

[0037] According to another embodiment, a material composition comprises an inductor alloy having carbon disposed within its metallic lattice. Preferably, at least some of the carbon is disposed at interstitial sites within the metallic lattice, and more preferably, the carbon is substantially uniformly dispersed within the metallic lattice. Furthermore, in some embodiments, the grain boundaries and / or surfaces of the material composition are substantially free of carbon aggregates and / or agglomerates. Therefore, the maximum identifiable feature size of the material composition can be in the range of about 0.1 nm to about 1 µm. At least some carbon atoms are covalently bonded to metal atoms in the metallic lattice, and the covalent bonds between the carbon atoms and the metal atoms are nonpolar covalent bonds or include nonpolar covalent bonds. In some embodiments, these covalent bonds may consist substantially of or entirely of nonpolar covalent bonds. Similarly, carbon atoms may be covalently bonded to other carbon atoms, and according to different embodiments, these covalent bonds may include nonpolar covalent bonds, consist substantially of nonpolar covalent bonds, or consist entirely of nonpolar covalent bonds. Therefore, the composition of one or more substances may substantially or completely lack polar covalent bonds. Similarly, a metal lattice may substantially or completely lack ionic bonds.

[0038] According to another embodiment, a material composition comprises a metal lattice having at least about 15 wt% carbon disposed therein. Preferably, at least some of the carbon is disposed at interstitial sites of the metal lattice, and more preferably, the carbon is substantially uniformly dispersed in the metal lattice. Furthermore, in some embodiments, the grain boundaries and / or surfaces of the material composition are substantially free of carbon aggregates and / or agglomerates. Therefore, the maximum identifiable feature size of the material composition can be in the range of about 0.1 nm to about 1 µm. At least some carbon atoms are covalently bonded to metal atoms of the metal lattice, and the covalent bonds between carbon atoms and metal atoms are nonpolar covalent bonds or include nonpolar covalent bonds. In some embodiments, such covalent bonds may consist substantially or entirely of nonpolar covalent bonds. Similarly, carbon atoms can be covalently bonded to other carbon atoms, and depending on the implementation, these covalent bonds can include nonpolar covalent bonds, consist substantially of nonpolar covalent bonds, or consist entirely of nonpolar covalent bonds. Therefore, the composition of one or more substances may substantially or completely exclude polar covalent bonds. Likewise, a metallic lattice may substantially or completely exclude ionic bonds.

[0039] In various embodiments of the foregoing configuration, the metal lattice may comprise one or more metals selected from the group consisting of: aluminum, copper, iron, nickel, titanium, tantalum, tungsten, chromium, molybdenum, cobalt, manganese, niobium, and combinations thereof. Therefore, the metal lattice may be characterized by a crystal structure such as face-centered cubic (FCC), body-centered cubic (BCC), or hexagonal close-packed (HCC). Furthermore, the metal lattice may contain approximately 15 wt% to approximately 90 wt% carbon (e.g., in various embodiments, approximately 20 wt%, approximately 25 wt%, approximately 33 wt%, approximately 40 wt%, approximately 50 wt%, approximately 60 wt%, approximately 75 wt%, or up to 90 wt%). Carbon is preferably present at interstitial sites within the metal lattice. In some methods, the metal may be present in alloy form. For example, in a particularly preferred method, the metal is present in the form of one or more Inconel high-nickel alloys, such as Inconel 600, Inconel 617, Inconel 625, Inconel 690, Inconel 718 and / or Inconel X-750. More preferably, the Inconel high-nickel alloy is a superalloy. [Overview]

[0040] This paper describes the integration of low-dose nanofiller carbon-based materials (such as graphene) with metals. Graphene is renowned for its inherent structural properties, such as high aspect ratio and "2D" planar geometry. Graphene possesses remarkably good mechanical, physical, thermal, and electrical properties due to its in-plane sp2 C=C bonds (which produce a 2D planar geometry). Therefore, compared to alternatives such as microfilled polyacrylonitrile (PAN)-based carbon fibers, graphene is an ideal reinforcement for metal matrix composites. It should be noted that even at low graphene nanosheet content (loading), 3D networks are formed with anisotropy (meaning that the values ​​of physical properties differ when measured in different directions), which significantly improves thermal and electrical conductivity as well as mechanical properties.

[0041] Challenges encountered in using carbon nanofillers in metal matrix composites include poor dispersion due to poor wettability (the ability of a liquid to maintain contact with a solid surface due to intermolecular interactions when the two are brought together; the degree of wettability (also known as wettability) is determined by the force balance between adhesive and cohesive forces). Due to the van der Waals forces between carbon atoms, the increased surface area of ​​the nanofillers causes particles to cluster and become entangled. Aggregation of nanofillers in metal matrix composites can lead to the formation of undesirable cracks and pores, potentially compromising the structural integrity of the resulting material and causing premature failure under high loads or performance conditions.

[0042] Although many processing methods, such as conventional powder metallurgy, hot rolling, casting, and additive manufacturing, have been (and may now be) used to produce metal matrix composites, challenges remain in achieving uniform dispersion of nanofillers. Some examples of the challenges encountered in attempting to achieve nanofiller dispersion include the damage to nanofillers caused by stress applied during consolidation and undesirable or uncontrollable chemical reactions with the matrix at high temperatures during sintering and casting.

[0043] Compared to the sides and ends of graphene sheets, which may more readily interact with metals to form carbides (which is thermodynamically favorable according to the Gibbs free energy), the defect-free basal surface of graphene exhibits exceptionally favorable chemical stability. However, defects can easily form in the basal surface during processing, leading to carbide formation and adversely affecting the properties of the composite material. Therefore, relatively harsh processing conditions such as high temperature and high pressure can negatively impact the interfacial quality between the carbon nanofiller and its surrounding metal matrix. Specifically, high temperature and high pressure can adversely affect wetting ability and structural integrity, potentially harmfully influence carbide formation, and may also induce other detrimental interfacial reactions.

[0044] An alternative process known as covetic (as described above) has been successfully used to incorporate carbon nanofillers into metal matrices. In covetic processes, it has been demonstrated that the network of graphene "ribbons" and nanoparticles, formed within liquid metal using an applied electric field, exhibits remarkable stability within the metal matrix, even after remelting. Consequently, this composite structure demonstrates higher thermal and electrical conductivity than the parent metal. [, Evenly dispersed , ] [, , ]

[0045] One of the challenges of incorporating graphene into a metal matrix is ​​achieving uniform dispersion. Covetic processing overcomes this problem by simultaneously exfoliating and wetting graphene ribbons and / or particles (from the decomposition of carbon electrodes or carbon additives) within an applied electric field. Impurities such as oxygen and hydrogen can be managed via redox reactions at the particle surface, assuming an appropriate induced voltage at that surface to promote wetting / dispersion. The challenges include controlling the structural integrity and uniformity of the graphene ribbons and / or particles (e.g., uniformity in size, defects, etc.), controlling their chemical reactivity with the metal at high temperatures, and controlling the distribution of particles within the melt and on its surface. [, Other complexities , ] [, , ]

[0046] While the fundamental energy conduction modes (both thermal and electrical) in metals can be (at least partially) carried out by electrons and controlled by the crystallinity and impurities of fillers such as graphene to enhance the thermal conductivity of metal matrix composites (where conduction occurs via phonons in graphene), a certain degree of matching and / or coherence with the metal lattice (otherwise or alternatively referred to as the scaffold, matrix, or structure) is required (e.g., bulk-bonded nanoscale carbon), or a minimum interlayer spacing (e.g., proximity or network) threshold is needed for conduction between sheets (e.g., graphene would need to be a single layer or only a few layers with a length of tens of nanometers). However, regarding reinforcing the metal matrix, for suitable load transfer (note that for maximum load transfer, the length of graphene can be greater than ~0.5 μm), graphene may need to be chemically bonded (or, in some cases, physically bonded) to the matrix. Besides solid solution strengthening relying on coherent and / or semi-coherent elastic strain between carbon (graphene) nanofillers and metal lattices, discrete graphene nanoparticles can serve as barriers to dislocation stacking or pinning at grain boundaries (such as Hall Petch grain refinement, a method of strengthening materials by changing the average crystallite (grain) size; this grain refinement is based on the observation that grain boundaries are insurmountable limits for dislocations and that the number of dislocations within a grain can affect the way stress is formed in adjacent grains, which will ultimately activate dislocation sources and thus allow deformation to occur in adjacent grains; therefore, by changing the grain size, the number of dislocations stacked at grain boundaries and the yield strength can be affected), both of which can improve mechanical performance.

[0047] Similarly, due to its 2D properties and high surface area, graphene can be aligned not only along the slip plane within the metal structure but also along the grain boundaries. Regardless of whether the properties of interest are chemical, mechanical, thermal, or electrical, the greater the alignment and matching (at the atomic level) between the nanofiller and the crystal structure of the surrounding metal matrix, the greater the enhancement and stability of the properties of the metal matrix composite structure.

[0048] Fundamentally, the growth of carbon at the metal surface (heterogeneous) or its precipitation from solution in the melt (homogeneous) depends on the solubility of carbon in the metal (according to the binary phase diagram shown on the right side of Figure 10). For example, near the melting point of the metal, the solubility of carbon in pure transition metals (generally, and many pure metals) is very low, but this solubility increases with increasing temperature well above the melting point of the metal (e.g., up to 2,000 °C and above). The solubility of carbon in nickel (e.g., near the hypereutectic point of about 2.5%) is among the higher solubility of carbon in pure metals. It should be noted that the addition of interstitial impurities (such as oxygen, boron, or nitrogen) or substitutional atoms to the metal can affect (e.g., potentially increase) the solubility of carbon. It has been shown that the higher the solubility of carbon in the metal or the higher the temperature of the molten metal, the thicker the carbon deposits at the metal surface as the metal cools and solidifies. It should be noted that carbon has a higher solubility near free surfaces, which, combined with the interfacial energy of the liquid-gas interface, facilitates the precipitation of solid carbon at the metal melt-air interface. The apparatus and the technique for operating the apparatus to overcome the problems associated with this phenomenon are described in connection with the accompanying drawings and discussion. [, Definitions and Diagram Usage , ] [, , ]

[0049] Some terms used in this specification are defined below for ease of reference. The terms presented and their individual definitions are not strictly limited to these definitions—a term may be further defined by its use in this disclosure. The term "illustrative" is used herein to mean serving as an example, instance, or illustration. Any form or design described herein as "illustrative" is not necessarily to be construed as superior or advantageous to other forms or designs. Rather, the use of the word "illustrative" is intended to present the concept in a concrete manner. As used in this application and the appended claims, the term "or" is intended to mean an inclusive "or," not an exclusive "or." That is, unless otherwise specified or clearly seen in the context, "X adopts A or B" is intended to mean either of the natural inclusive arrangements. That is, if X adopts A, X adopts B, or X adopts both A and B, then "X adopts A or B" is satisfied in any of the foregoing cases. As used herein, "at least one of A or B" means at least one of A or at least one of B, or at least one of both A and B. In other words, the phrase is disjunctive. The articles "a" and "an" used in this application and the appended claims should be generally interpreted as "one or more" unless otherwise specified or clearly indicated from the context to refer to the singular form.

[0050] This document describes various embodiments with reference to the accompanying drawings. It should be noted that the drawings are not necessarily drawn to scale, and throughout the drawings, elements with similar structures or functions are sometimes indicated by similar reference numerals. It should also be noted that the drawings are intended only to facilitate the description of the disclosed embodiments—the drawings do not represent an exhaustive treatment of all possible embodiments and are not intended to limit the scope of the claims in any way. Furthermore, the illustrated embodiments are not required to depict all forms or advantages used in any particular environment.

[0051] The features or advantages described in connection with a particular embodiment are not necessarily limited to that embodiment and may be practiced in any other embodiment, even if not stated so. References to "some embodiments" or "other embodiments" in this specification mean that a particular feature, structure, material, or characteristic described in connection with that embodiment is included in at least one embodiment. Therefore, the phrases "in some embodiments" or "in other embodiments" appearing in different places in this specification do not necessarily refer to the same one or more embodiments. The disclosed embodiments are not intended to limit the scope of the claims. [Description of exemplary implementation methods]

[0052] Figure 1A is a comparative table 1A00 showing two different covetic material forming techniques 102 and exemplary materials produced by applying each of these covetic material forming techniques.

[0053] In conventional metal melting method 103 used to produce covetic materials, solid carbon is added to the molten metal. This conventional metal melting technique is governed by the kinetics of carbide formation and interdiffusion across the solid-liquid (such as carbon-metal) interface under an applied current, which provides additional energy to overcome the stacking fault energy between carbon and metal atoms. Thus, conventional metal melting techniques for forming covetic processes are not significantly different from other composite material processing methods (such as powder metallurgy and / or hot rolling), which involve consolidating second-phase particles into a metal matrix. These conventional composite material processing methods face many challenges in terms of dispersion and / or distribution, reactivity, and variability of material properties. Furthermore, conventional covetic processing relies on batch processing and often produces inconsistent conversion yields and wide variations in the resulting properties.

[0054] As depicted in image 105, when conventional metal melting method 103 is used, the resulting material comprises numerous carbon aggregates and / or agglomerates, particularly at grain boundaries and / or the surfaces of the metal lattice. This subsequently: (1) limits the effect of carbon in reinforcing the lattice; and (2) limits the tunability of surface functionalization morphologies. In contrast, when the currently disclosed technique is used, the resulting material exhibits almost uniform homogeneity (e.g., the absence or substantial absence of aggregates and / or agglomerates, particularly at grain boundaries and / or the surfaces of the lattice), which arises from the uniform dispersion of carbon within the lattice. This is shown in homogeneity image 106.

[0055] The characteristics of the covetic material depicted in homogeneous image 106 can be found in many desired material properties 108, such as uniformity, high carbon loading, and low carbon content at the surface. These are highly desired material properties that are not exhibited by materials formed using conventional metal melting method 103. Therefore, what is sought is an improved method to overcome the shortcomings of conventional metal melting method 103.

[0056] One such improved method relates to plasma spraying torch method 104. The application of the plasma spraying torch method results in a consistent yield of covetic materials, thus overcoming the yield disadvantages of conventional metal melting methods. Furthermore, the covetic materials produced using the plasma spraying torch method possess the aforementioned improved mechanical properties, improved thermal properties, and improved electrical properties, thus overcoming the disadvantages of materials obtained by conventional metal melting methods. [, Improved methods , ] [, , ]

[0057] As shown, plasma spraying torch method 104 can be configured to use introduced input materials (referring to carbon-containing raw materials provided in gaseous form, such as methane, and powered by applying MW of energy guided through the methane gas, etc.). However, by dissociating carbon-containing gases (such as methane or other hydrocarbon sources) at high temperatures, self-limiting monolayers of carbon—particularly pristine graphene—can be grown on or within metal lattices (such as copper, gold, zinc, tin, and lead). The number of monolayers depends at least in part on the solubility of carbon in the metal. The growth kinetics, bonding, and final structure of graphene films on metal substrates depend on the valence electrons and symmetry (close-packed planes) of the metal. Similarly, metals can be grown on carbon, preferentially nucleating and growing at carbon defect sites or also at selective oxygen or hydrogen termination sites. Alternating stacks of monolayers of carbon and metal can then be fabricated to achieve the reinforcing properties of graphene-reinforced metal composite structures.

[0058] Using a microwave plasma reactor, pristine 3D few-layer graphene particles can be continuously nucleated and grown from a hydrocarbon gas source. Furthermore, by adding selective elements to the plasma gas stream, these selective elements can be incorporated into the 3D graphene particle scaffold. The microwave plasma reactor process provides a unique reaction environment in which gas-solid reactions can be controlled under non-equilibrium conditions (e.g., chemical reactions can be independently controlled by ionization potential and momentum, as well as thermal energy). Reactants can be inserted into the plasma reactor region in solid, liquid, or gaseous form to independently control the nucleation and growth kinetics of unique non-equilibrium structures (e.g., graphene on metal and metal on graphene).

[0059] For example, to produce nanoscale integrated graphene-metal composites, fine nanoscale metal particles can be introduced into a microwave plasma torch along with hydrocarbon gases (such as methane). The methane dissociates into hydrogen and carbon (e.g., C and H2 are formed using the ideal energy of microwave plasma), which then nucleates and grows ordered graphene onto the semi-molten surface of the metal particles. Non-equilibrium energy conditions can be generated by adjusting process conditions to independently control the temperature of the metal relative to carbon reactivity and delivery to the metal surface. At controlled low energies, ionized hydrogen (or other ions) can be used to bombard / sputter the growing graphene-metal surface without destroying the structure of the graphene-metal composition. This subsequently promotes further growth of alternating graphene-metal layers. Furthermore, depending on the residence time and energy within the plasma reaction region, metal-graphene structures with specific properties can be produced, which are retained when the metal-graphene structure is sprayed onto a substrate at a controlled temperature and then rapidly cooled. The controlled energy formation of metal-graphene structures within plasma and the control of substrate temperature provide independent control over energy conditions throughout the evolution of these covetic materials.

[0060] Graphene can be applied (and / or deposited) onto metal or metal-containing material layers via sputtering (the phenomenon where microscopic particles of a solid material are ejected from its surface after being bombarded by high-energy particles of plasma or gas; the fact that sputtering can be applied to extremely fine material layers is frequently utilized in science and industry—in which sputtering is used to perform precise etching, analytical techniques, and to deposit thin film layers in the manufacture of optical coatings, semiconductor devices, and nanotechnology products). When used with the MW plasma reactor discussed here, this sputtering, as described above, can be controlled to promote the growth of alternating graphene-metal layers by controlling the residence time and energy within the plasma reaction region. These alternating graphene-metal layers are organized in coherent planes of atoms with a regular (such as crystalline) configuration. When the graphene-metal layer is rapidly quenched (in materials science, quenching or rapid / abrupt quenching refers to the controlled rapid cooling of a workpiece in water, oil, or air to obtain certain material properties; quenching is a heat treatment that prevents or controls unwanted cryogenic processes, such as phase transitions, by reducing the time window during which such unwanted reactions are thermodynamically advantageous and kinetically feasible; for example, quenching can reduce the grain size of both metallic and plastic materials, thereby increasing their hardness) onto a cooler substrate, the crystal configuration is preserved. As described, rapid quenching is used to essentially "freeze" (meaning to maintain a substantially solid state, not just the traditional definition of a liquid-to-solid phase transition) the graphene to a metal in the desired crystal configuration formed in a plasma reactor. The resulting material exhibits highly uniform homogeneity both internally and at its surface. This highly uniform homogeneity can be used to distinguish it from materials already formed using the metal melting method 104. The reason is that the metal melting method 104 cannot control the ion energy independently of thermal energy. More specifically, because the metal melting method 104 cannot achieve the desired higher ion energy independently of thermal energy, the temperature in the metal melting reaction chamber may be too high to allow the graphene-metal layer to be organized in the atomically coherent plane with the desired crystal configuration.

[0061] Therefore, when using metal melting method 104, the desired crystal structure of the graphene-metal layer will never appear, and thus the desired crystal structure cannot be retained when the graphene-metal layer is quenched onto a cooler substrate. Instead, when using metal melting method 104, undesirable carbon precipitation occurs (such as carbon precipitating out of the melt), which in turn leads to the undesirable formation of aggregates and / or agglomerates, resulting in inhomogeneity of the resulting composition. This inhomogeneity of the resulting composition may lead to less than ideal chemical and / or physical (mechanical) properties, including but not limited to premature mechanical failure.

[0062] Figure 1B presents a high-resolution transmission electron microscopy image 114 and a high-resolution energy-dispersive X-ray image 116. For convenience, the homogeneous image 106 of Figure 1A is also shown here.

[0063] As depicted in this set of illustrative images, carbon is uniformly distributed within the metal lattice. This is emphasized in high-resolution transmission electron microscopy image 114. Furthermore, the extremely high carbon loading within the metal lattice is clearly shown in high-resolution energy-dispersive X-ray image 116. In this example, the carbon loading forms approximately 60% of the entire copper-carbon lattice. This is shown in high-resolution energy-dispersive X-ray image 116. In this particular image, the darker areas represent carbon, and the brighter areas (displayed as dots) represent copper.

[0064] As can be seen from the images, and specifically from the pattern of the high-resolution energy dispersive X-ray image 116, the carbon and the parent metal (such as copper in this case) are uniformly dispersed. As shown, this uniform lattice-level dispersion exists at the surface and also deep within the parent metal. Figures 20A1, 20A2 and 20B provide further images of the covetic material, which follow (1) the material evolution process, (2) the plasma spraying torch equipment and (3) the discussion of various configurations of the plasma spraying torch.

[0065] In one application scenario, the covetic material in Figure 1B can be fabricated using a tunable microwave plasma torch, which produces integrated graphene-metal composite films at high rates and volumes. A specific manufacturing process will now be briefly discussed, during which graphene is grown onto small molten metal particles.

[0066] Figure 2 illustrates a manufacturing process 200 for growing graphene onto small molten particles. Alternatively, manufacturing process 200, or any variant thereof, may be implemented within the architectural and functional context of the embodiments described herein. Manufacturing process 200, or any variant thereof, can be implemented in any environment.

[0067] One possible approach is to use a microwave plasma torch with "unbalanced energy" to provide unbalanced control of the metal temperature, independent of carbon production. This plasma torch energy is then directed to the surface of molten and / or semi-molten metal particles. This technique allows time for growth on the melt. The growth on the melt (or semi-molten material or core-shell material) generated within the torch flows out via a main plasma plume to the metal surface on which growth will take place, and is subsequently rapidly quenched. This technique provides a means for growing thick films, which, in delamination, can be grown into homogeneous ingots and / or grown to be post-processed or remelted into components for application.

[0068] Additionally, Figure 2 is presented to illustrate the effects of independently controlling the temperature of the constituent materials and the gas-solid reaction chemistry when growing graphene onto small molten particles. Figure 2 shows the evolution through several covetic material manufacturing processes; and presents the process used in the formation of plasma torch-based covetic materials.

[0069] As shown, semi-solid particles exiting the plasma torch can be deposited onto a temperature-controlled substrate in an addition-layer manner. Unlike standard plasma torches, which are limited in terms of operating flow rate, power control, and other configurations, the microwave plasma torch in question can be operated to independently control the temperature of the constituent materials and the gas-solid reaction chemistry.

[0070] As can be seen from the above disclosure, microwave plasma sources can produce, for example: (1) higher plasma density; (2) ion energy with a narrower ion energy distribution; and (3) improved coating properties. This is at least partly attributed to improved power coupling and (electromagnetic) absorption at 2.45 GHz. Typical pressure-dependent electron temperatures are on the order of 1 eV to 15 eV, resulting in plasma densities > 10¹¹ cm⁻³. Such low electron temperatures are advantageous not only in controlling plasma chemistry but also in limiting ion energy, where the ion energy of argon-based coaxial microwave plasma is typically in the range of 5 eV to 80 eV. The narrow plasma sheath formed by using such high-density plasma prevents collisional broadening of the ion energy distribution, thus resulting in a sharp ion energy distribution that supports fine control over certain film deposition processes. In addition, non-equilibrium energy can be formed and controlled by applying pulsed power to microwave plasma. During the application of microwave energy, power is delivered throughout the volume of plasma to be formed, thus energy accumulates in a progressive collisional energy pattern.

[0071] Figure 2 was previously discussed and includes techniques for applying microwave energy power, which are further detailed below.

[0072] Figure 3 depicts a plasma energy state table 300 illustrating how a pulsed microwave energy source can be used to grow graphene onto small molten particles.

[0073] Microwave plasma sources have the potential to achieve higher plasma densities, narrower ion energy distributions, and improved coating properties due to improved power coupling and absorption at 2.45 GHz. Typical pressure-dependent electron temperatures are on the order of 1 eV to 15 eV, resulting in plasma densities > 10¹¹ cm⁻³. Such low electron temperatures are advantageous not only for controlling plasma chemistry but also for limiting ion energy, with ion energies in argon-based coaxial microwave plasmas typically ranging from 5 eV to 80 eV. The narrow plasma sheath formed by this high-density plasma prevents collisional broadening of the ion energy distribution, resulting in a sharp ion energy distribution, which is necessary for fine control in some film deposition processes. Furthermore, non-equilibrium plasma energy can be formed and controlled by using pulsed power delivered to the microwave reactor. During microwave energy application, power is delivered throughout the volume of plasma to be formed, thus accumulating energy in a progressive collisional energy pattern.

[0074] Once the initial plasma has formed over most of the volume, the delivery antenna, where the energy is at its maximum, continues to increase in a highly localized manner. The plasma density in the vicinity decreases slightly until the plasma contracts. Further details regarding the general methods for manufacturing and using pulsed microwave energy sources are described in U.S. Patent Publication No. 10,332,726, published June 25, 2019, which is hereby incorporated by reference in its entirety.

[0075] Figure 3 illustrates that the initial energy of the plasma is much higher in the non-equilibrium state until the plasma contracts to a much lower stable temperature. More specifically, the plasma energy state diagram depicts the transition from the initial high-energy non-equilibrium state to a lower-energy stable equilibrium state. Once the initial plasma has formed, the delivery antenna, with its maximum energy, will continue to increase in a highly localized manner until the plasma contracts and is lost in the rest of the chamber due to energy shielding.

[0076] A controllable pulsed microwave energy source can be used to optimize the electron temperature for growing graphene onto small molten particles. This is particularly effective at pressures >>20 Torr. The chamber environment must be controlled to ensure homogeneous plasma chemical dissociation and a homogeneous material coating.

[0077] As shown in Figure 3, the energy curve indicates a high initial energy level that contracts to a lower level after a period of time and remains there until power is removed. The plasma extinguishes and, upon restarting, follows the energy cycle again. By shortening the time between initial plasma ignition and its stabilization, the plasma is primarily retained within the system body, where more homogeneous material dissociation may occur. This shortening of the time between initial plasma ignition and stabilization can be achieved by controlling the pulse frequency and duty cycle.

[0078] Figure 4 illustrates and describes a technique for controlling the electronic temperature in a pulsed microwave reactor.

[0079] Figure 4 illustrates an electronic temperature control technique 400 for growing graphene onto small molten particles. Alternatively, electronic temperature control technique 400, or any one or more variations thereof, may be implemented within the architectural and functional context of the embodiments described herein. Electronic temperature control technique 400, or any such embodiment thereof, can be implemented in any environment.

[0080] Figure 4 illustrates the state of growing several layers of graphene onto molten nanoscale particles, rather than mixing carbon into the molten slurry bulk. Specifically, the figure shows the contribution of controlling the microwave pulse frequency to controlling the plasma temperature. [, Plasma temperature control via control pulse frequency , ] [, , ]

[0081] As depicted in Figure 3 above, the energy curve shows a high initial energy level that contracts to a lower level after a period of time and remains there until the power is removed. The plasma extinguishes and, upon restarting, follows the energy cycle again. By shortening the time between initial plasma ignition and reaching steady state, the plasma is primarily retained within the system bulk, where more homogeneous material dissociation may occur.

[0082] As shown in Figure 4, the effect essentially depends on the timing of the microwave energy source's on / off cycle. By controlling the pulse frequency, optimal chemical dissociation and a uniform coating can be produced. Furthermore, the average temperature of the plasma can also be controlled by setting the pulse frequency. [, Plasma temperature control in microwave plasma torch , ] [, , ]

[0083] This paper discusses an integrated microwave plasma torch for the formation of integrated second-phase carbon-metal composite structures, which exhibit enhanced mechanical, thermal, and electrical properties compared to existing metal alloy and conventional composite material processing methods. Furthermore, the microwave plasma torch can be used to directly form carbon-metal composite coatings and particles onto high-value asset components. In addition, the aforementioned methods and equipment meet many clean energy goals related to improved power distribution and efficient transformer and heat exchanger performance. [, Practical applications of microwave plasma torch , ] [, , ]

[0084] Using integrated microwave plasma torch technology, materials can be deposited and / or formed at faster rates and cost-effectively, and can be applied in a variety of configurations. Contributors to this technology include various energy production industries, particularly those related to transmission and storage transportation, military equipment, and many other manufacturing sectors. As a concrete example, the metallic surfaces of aircraft can be treated with plasma spraying to create covetic materials at the metal-air interface. This makes the metallic surface resistant to corrosion. Furthermore, the carbon atoms near the surface allow other materials to chemically bond to the carbon atoms and / or adhere to the surface. The aforementioned other materials that can be chemically bonded to the carbon atoms can be selected based on the requirements of various practical applications.

[0085] As another concrete example of practical application, the metal surfaces of air vehicles (such as airplanes, helicopters, drones, projectiles, missiles, etc.) can be treated with plasma spraying to produce a covetic material coating that acts as an infrared shield (such as a detection countermeasure).

[0086] Figure 5 illustrates a dual plasma torch apparatus 500 for growing graphene onto small molten particles. Alternatively, the dual plasma torch apparatus 500, or any of its variants, may be implemented within the architectural and functional context of the embodiments described herein. The dual plasma torch apparatus 500, or any of its variants, can be implemented in any environment.

[0087] The apparatus shown is equipped with: (1) a metal plasma spraying torch for supplying molten metal to the surface of a heated substrate (Al, Cu, Ag, etc.); and (2) a microwave plasma torch for delivering ionized carbon and plasma radicals to the molten surface so that covetic growth can be achieved on the molten metal.

[0088] The system is inserted into an inert gas environment or a controlled atmosphere chamber to provide better control over the oxidation of the material. In one embodiment, the setup and operation of the torch in Figure 5 are shown in Table 1, the details of which are discussed below. step Setup and Operation Description 1 Identification and selection of reactant materials 2 Integrates standard non-microwave plasma spraying torches and microwave plasma torches into a dual plasma torch. 3 Define plasma torch processing parameters 4 Operate dual plasma torches to generate graphene growths on the surface of semi-molten particles. Table 1 [, step , ] [, D1 , ] [, Identification and selection of reactant materials , ] [, , ]

[0089] Plasma spraying can be performed simultaneously with any amount of metal and metastable carbon materials to form nano-carbon-metal composite structures. When forming 2D graphene at concentrations above the thermodynamic solubility limit, different metals with high electrical and thermal conductivity can be used. In some cases, two different metals are selected, each with different carbon solubility limits and / or different melting points and / or different densities and / or different crystal structures. [, step , ] [, D2 , ] [, Microwave and , ]「 [, standard , ]” [, Selection, modification and verification of plasma spraying torch , ] [, , ]

[0090] The apparatus of Figure 5 may (in some embodiments) consist substantially of a "standard" off-the-shelf plasma spraying and microwave plasma torch. Having two torches allows for two distinct processing steps: (1) initial melting of the metal; and (2) nucleation / growth of graphene flakes from a hydrocarbon source. Each of the two torches can be controlled independently of the other.

[0091] As shown in Figure 5, two torches are positioned side-by-side for parallel or sequential operation. Specifically, a microwave plasma with low electron temperature and high electron density can be used to optimize graphene formation (including nucleation rates below the carbon supersaturation threshold), while a standard plasma spraying torch can be used to heat metal powder / particles to a molten or semi-molten state and then accelerate the particles (and nucleated ionized carbon / graphene) toward the substrate. Two independent flow streams can be coordinated to achieve fine-scale graphene growth on the surface of semi-molten particles. In some cases, the dual-torch configuration includes components for maintaining an inert atmosphere (such as a covering gas) in or near the torch exit flow and in and around the impact zone on the substrate surface. This arrangement is advantageous in minimizing or preferably preventing the inclusion of atmospheric gases (such as oxygen, nitrogen, water vapor, etc.) in the material composition, as will be understood by those skilled in the art, which may adversely affect the bonding between carbon and metal atoms. Therefore, in some embodiments, the dual-flame system is configured to be inserted into a fully controlled inert gas environment (such as a chamber) to provide effective control over the oxidation of the material. [, step , ] [, D3 , ] [, Basic Principles and Definitions of Plasma Machining Parameters , ] [, , ]

[0092] Reactants (such as hydrocarbons) and inert gases and flow patterns are selected to ensure plasma stability and to control nucleation and growth processes within the plasma (e.g., given gas mixtures and supersaturation thresholds). The acceleration rate and temperature of metastable carbon are controlled during the plasma's migration to the substrate. Correspondingly, standard plasma spraying torch process conditions are set to produce a solidified film on which carbon can impact and react. Surface temperature and local gas phase environment are controlled to promote the interaction and growth of the metastable carbon phase. [, step , ] [, D4 , ] [, Dual operation , ] [, ( , ] [, Metals and microwaves , ] [, ) , ] [, Plasma torch , ] [, , ]

[0093] Various processing window parameters of the metal and microwave plasma torches are configured to be controlled independently, or in some embodiments, in combination. The processing window for integrated carbon-metal formation is characterized before, during, and after the operation of one or more of the metal and microwave plasma torches (referred to herein as "dual plasma torches"). Furthermore, one or more parameters or combinations thereof are selected to observe carbon-metal deposition, and the deposited sample can be characterized with respect to various distinguishing factors using any techniques known in the art, including (but not limited to): morphology (such as using scanning electron microscopy (SEM)), structure (such as via X-ray diffraction (XRD) and Raman spectroscopy), and / or physical and chemical composition.

[0094] Figure 6 illustrates a pulsed microwave plasma spraying torch apparatus 600 that can be adapted for growing graphene onto small molten particles. As an example, one or more variations of the pulsed microwave plasma spraying torch apparatus 600 (or any form thereof) can be implemented within the architectural and functional context of the embodiments described herein. The pulsed microwave plasma spraying torch apparatus 600 (or any form thereof) can be implemented in any environment.

[0095] In this configuration, the transverse electric field (TE) microwave energy power component may be coupled to (or, in some embodiments, substantially penetrate) the central dielectric tube to propagate microwave energy into and through it. The gas supplied to the central region (in this example) may be a hydrocarbon gas that absorbs microwave radiation, such as methane. Metal powder (carried by a substantially inert carrier gas) is supplied to be heated within the body (or main chamber) of the pulsed microwave plasma spraying torch apparatus 600 by a combination of plasma-derived and applied thermal energy. Upon exposure to this energy, the metal powder melts upon reaching its melting temperature to produce a viscous, flowable liquid material or droplets (possibly containing semi-solid materials), or any other conceivable dispersion (largely depending on the accompanying melting conditions).

[0096] When hydrocarbon gases decompose into their constituent elements, carbon radicals nucleate on the exposed surface of molten metal droplets. The combination of microwave energy tuning settings and thermal plume temperature settings allows for different temperatures between the melting temperature and the plasma decomposition / ionization temperature in the central region of the pulsed microwave plasma spraying torch 600. Non-equilibrium conditions (temperature, pressure, etc.) within the central chamber or region of the plasma spraying torch allow (or otherwise promote) the internal lattice placement of graphene / carbon, while rapid quenching creates conditions favorable for covetic material growth.

[0097] As understood herein, internal lattice placement refers to the positioning of a synthetic lattice structure of a carbon material (such as graphene) within the lattice structure of an input metal, such that individual carbon and metal atoms are at least partially aligned. For example, internal lattice placement includes one or more graphene layers (preferably coherent planar layers) (such as single-layer graphene (SLG) or few-layer graphene (FLG)) spaced together between the basal planes of the metal lattice and / or spaced apart and interleaved between the basal planes of the metal lattice. Internal lattice placement also includes embodiments of other carbon-based compounds (such as three-dimensional graphene, carbon nano-onions (CNO), graphene nanoribbons, carbon nanotubes, graphene superlattices, and their equivalents as will be understood by those skilled in the art) spaced together between the basal planes of the metal lattice and / or spaced apart and interleaved between the basal planes of the metal lattice. Similarly, regardless of the specific synthetic lattice structure of the carbon-based compound, the key characteristic of internal lattice placement is that individual carbon and metal atoms are at least partially aligned. A diagram showing an internal lattice in which the carbon lattice and the metal lattice are oriented such that the carbon atoms and the metal atoms are at least partially aligned is presented in Figures 8A-B, 12, 26C and 26D and the corresponding written descriptions below.

[0098] Internal lattice placement therefore refers to the spatial arrangement of carbon and metal atoms in the lattice and is distinct from chemical and / or ionic bonding. However, according to various embodiments, the innovative material composition described herein may additionally include several characteristics, such as nonpolar covalent bonding between individual carbon atoms in the material composition and / or nonpolar covalent bonding between individual carbon atoms and metal atoms in the material composition.

[0099] Preferably, the composition exhibiting internal lattice placement is characterized by a substantial lack of polar covalent bonds between individual carbon atoms and a substantial lack of polar covalent bonds between carbon atoms and metal atoms. More preferably, the inventive concept described herein is characterized by a substantial lack of ionic bonds within the metal lattice.

[0100] As those familiar with this technology will understand, polar covalent bonds, nonpolar covalent bonds, ionic bonds, and metallic bonds each have unique distinguishing characteristics, as well as corresponding electronic and chemical properties.

[0101] An ionic bond is formed after the bonding electrons are completely transferred from one atom to another. The resulting positively and negatively charged ions are then electrostatically attracted. Importantly, ionic bonds rarely have any particular directionality because they are formed by each ion being electrostatically attracted to all surrounding ions of opposite charge. Ionic compounds generally have high melting and boiling temperatures and are brittle (low mechanical strength), and are conductive in the molten state or in aqueous solutions.

[0102] In metallic bonding, the bonding electrons are nonlocalized on the atomic lattice. In metals, each atom provides one or more electrons residing between many atomic centers. The free movement of these nonlocalized (or "free") electrons thus leads to important properties of metals, such as high electrical and thermal conductivity. Notably, the innovative material compositions described herein, having carbon dispersed in a metal lattice and substantially covalently bonded between carbon atoms and metal atoms in the lattice, are characterized by the involvement of all or substantially all (e.g., at least 90%, at least 95%, at least 98%, at least 99%, etc.) of the electrons in such covalent bonds, thereby altering the electrical and / or thermal conductivity of the composition.

[0103] While both polar and nonpolar covalent bonding involve electron sharing, compounds that include polar covalent bonds are characterized by the unequal sharing of electrons among bonding partners. For example, in hydrogen chloride, the chlorine atom has a higher electronegativity than hydrogen and exhibits a stronger attraction for electrons. Therefore, the "shared" electrons are more strongly associated with the chlorine atom, resulting in a partially negative charge on chlorine and a partially positive charge on hydrogen (thus creating a dipole in the HCl molecule). In water, the bond between each hydrogen atom and oxygen atom is similarly characterized by the greater electronegativity of oxygen. This results in a dipole moment between each hydrogen atom and oxygen atom, and due to its curved shape, an entire dipole across the entire water molecule. However, not all compounds exhibiting nonpolar covalent bonding exhibit an entire dipole. Tetrachloromethane has four chlorine atoms bonded to a central carbon atom and equidistant from each other. Although each carbon-chlorine covalent bond is nonpolar, the spatial arrangement of the molecule eliminates the overall bond moment, resulting in a molecule with zero net polarity. Similarly, the linear shape of carbon dioxide eliminates the dipole moment exhibited between each oxygen atom and the central carbon atom, resulting in a molecular structure without a net dipole moment.

[0104] Regardless, in the presence of an electric field, the atomic and / or electron clouds involved in polar covalent bonding can shift, resulting in polarization aligned with the electric field. This phenomenon can give the corresponding compound energy storage capacity and contribute to the capacitance of the composition. Compounds exhibiting polar covalent bonding, especially small molecules or molecules having a majority of polar covalent bonds (e.g., at least 10%, at least 20%, at least 25%, at least 50%, etc. in various embodiments), are characterized by melting and boiling temperatures lower than those of compounds exhibiting ionic bonding (again, especially small compounds and compounds having a majority of ionic bonds), but higher than those of compounds exhibiting nonpolar covalent bonding (again, especially small compounds and compounds having a majority of nonpolar covalent bonds). Compounds exhibiting polar covalent bonding may or may not exhibit conductivity, but is generally less than that of ionic compounds. In addition, compounds exhibiting polar covalent bonds (especially small compounds and compounds that exhibit most polar covalent bonds) are moderately soluble in water (the solubility depends on the overall polarity of the compound), but are usually insoluble or only nominally soluble in nonpolar solvents.

[0105] Conversely, nonpolar covalent bonding is characterized by the equal sharing of electrons among the bonding partners, and therefore the absence of any dipole moment. Compounds that exhibit only (or substantially only) nonpolar covalent bonding between their constituent atoms thus lack the entire dipole moment, and lack the corresponding properties described above and other properties that a person generally skilled in the art will understand after reading this disclosure. Exemplary, non-limiting compounds that exhibit only (or substantially only) nonpolar covalent bonding include graphite, single-layer graphene (SLG), few-layer graphene (FLG), three-dimensional graphene, carbon nano-onions (CNO), graphene nanoribbons, carbon nanotubes (CNTs) (single-walled (SWCNTs) and multi-walled (MWCNTs)), graphene superlattices, etc., as described herein, and their equivalents that a person generally skilled in the art will understand after reading this specification.

[0106] For example, compounds exhibiting nonpolar covalent bonds (especially small molecules such as carbon dioxide, molecular hydrogen, and methane) and compounds that substantially do not contain polar covalent and ionic bonds are generally characterized by low boiling and melting temperatures and low electrical conductivity. In most compounds exhibiting nonpolar covalent bonds, the London dispersion force controls the electronic properties of the compound. However, although essentially composed of nonpolar covalent bonds, graphene (and similar compounds that exhibit sp2 and / or sp3 bonds and / or substantial coordination between electrons due to the physical arrangement and bonding mode of their molecular structure, as those skilled in the art will know after reading this disclosure) exhibits significant electrical conductivity. Similarly, compounds exhibiting nonpolar covalent bonds are generally insoluble in water or only nominally soluble in water (but soluble in nonpolar solvents).

[0107] Referring now to Figure 6, the single integrated microwave plasma torch in Figure 6 can be set up and operated as described in Table 2 below, the details of which are described below. step Settings / Operation Description 1 Deploy a single integrated microwave plasma torch 2 Operating a single integrated microwave plasma torch to form graphene-supported metal composite alloys 3 Characterization results Table 2 [, , ] [, step , ] [, S1 , ] [, Deploy a single integrated microwave plasma torch , ] [, , ]

[0108] Figure 6 depicts a single integrated microwave plasma torch. This torch has the capability to vacuum process solid, liquid, and vapor reactant raw materials using, for example, a small inert gas or a differential pump for controlling gas flow. The torch can be deployed in any environment (laboratory, research institution, or large-scale industrial enterprise, etc.). [, step , ] [, S2 , ] [, : Manipulating a single integrated microwave plasma torch to form graphene-supported metal composites , ] [,( , ]「 [, covetic , ]” [, ) , ] [, alloy , ] [, , ]

[0109] Microwave energy is delivered in a collinear waveguide configuration along with a centralized gas feed system for effective microwave energy absorption. The microwave energy source is used to heat the metal to a semi-molten state. When CH4 (or other hydrocarbon sources) decomposes (as its constituent substances) within the exhaust plume guided into the surface wave plasma gas dissociation tube, carbon radicals can nucleate on the surface of the metal droplets (e.g., in an organized, layer-by-layer manner) by being excited by plasma radicals (guided onto the metal droplets). The microwave thermal plume temperature and plasma energy tuning allow for independent control of the temperature between melt and plasma decomposition / ionization occurring in the central region of the pulsed microwave plasma spraying torch apparatus 600.

[0110] Measuring and optimizing process conditions. The desired process conditions are controlled by an integrated microwave plasma torch or by controlling the integrated microwave plasma torch to directly form graphene-loaded metal composites within a single-stage or multi-stage plasma torch. The plasma torch can modulate different regions of the surface wave plasma to increase the number of resonances (modulations) and optimize the formation of the target metal-carbon structure.

[0111] In addition to the process gas port shown at the depicted location (such as 605 for introducing hydrocarbon process gas), additional ports 604 may be provided at different locations. These additional ports can be used to control how process gases are introduced into the microwave field, and to introduce other process gases. For example, the process gas may be SiH4 or NH3. In some embodiments, more than one gas input port or more than one particle input port (such as a carbon input port and a metal input port) may be included, wherein the input ports may be located in different regions of the plasma torch.

[0112] The above settings and conditions, along with other conditions, were optimized to create conditions at the substrate surface that allow the impacting particles to solidify into a film. The deposited film was analyzed and characterized according to the method outlined in step S3 below. [, step , ] [, S3 , ] [, :verify , ] [, / , ] [, Characterizing graphene , ] [, ( , ] [, Second phase , ] [, ) , ] [, Metallic properties , ] [, , ]

[0113] Characterization of deposited, integrated carbon-metal composite structures is accomplished using several techniques. For example, X-ray photoelectron spectroscopy (XPS) and / or SEM-EDS can be used to determine chemical composition, binding energy (nanoscale carbon detection), and distribution. Furthermore, energy-dispersive X-ray spectroscopy (EDS) and / or SEM and / or Raman spectroscopy and / or XRD can be used to determine morphology and / or measure grain size and structural characteristics. The electrical and thermal properties of the composite material, as well as its tensile strength and modulus, can be evaluated using any known technique. [, result , ] [, , ]

[0114] The aforementioned technology utilizes a microwave plasma torch to continuously fabricate metal matrix composites. The process involves material nucleation and the formation of growth regions within the plasma, followed by accelerated and impact zones for consolidating the material onto a substrate. Each zone offers unique control over the synthesis / blending and integration of different materials; that is, the selectivity and unique blending of alloy particles within the plasma. Then, through controlling the momentum (primarily kinetics) and thermal energy during impact with the substrate, a unique additive process is implemented to control consolidation parameters such as porosity, defect density, residual stress, chemical and thermal gradients, phase transitions, and anisotropy.

[0115] Various materials were selected for use across a wide range of growth dynamics within plasma operating environments. Specifically, hydrocarbon gas sources with specific carbon-oxygen-hydrogen ratios and solid metal (or metal alloy) particle sources with different carbon solubilities, melting points, and crystal structures can be processed via pulsed energy plasma torch processing systems. In this way, specific plasma processing parameters can be identified based on the initial surface melting of the particles, along with the nucleation and / or growth and incorporation of 2D graphene and re-sputtered metal on the metal surface.

[0116] After graphene is incorporated into a metal using a microwave plasma torch, the "covetic-like" properties of the deposited material / film are characterized. As examples, these covetic-like properties may be characterized as (e.g.): (1) chemical composition (e.g., for detecting impurities and for detecting carbon forms); (2) carbon distribution (e.g., interstitial—referring to the location of carbon atoms or matter within the metal matrix or lattice, intragranular and intergranular); (3) electrical conductivity; and (4) the mechanical strength of the material. Characterization may include a comparison between the graphene-loaded and unalloyed parent metal. Furthermore, by way of example only, using a microwave plasma torch, the deposited material may exhibit a carbon-to-metal ratio in the range of approximately 3% to 90% (inclusive). In some cases, the carbon-to-metal ratio is in the range of approximately 10% to approximately 40% (inclusive). In some cases, the carbon-to-metal ratio is in the range of approximately 40% to approximately 80% (inclusive). In some cases, the carbon-to-metal ratio is in the range of approximately 80% to approximately 90% (inclusive). In some cases, the carbon-to-metal ratio is greater than 90% (including the extreme values). The carbon-to-metal ratio can be affected (or further affected) by parameters or specifications that define the coating process (such as temperature, thickness, homogeneity, etc.).

[0117] Therefore, carbon can be present in amounts that are not achievable with conventional techniques. For example, according to various embodiments, the resulting material may contain more than about 6 wt% carbon, more than about 15 wt% carbon, more than about 40 wt% carbon, more than about 60 wt% carbon, or up to about 90 wt% carbon. In various embodiments, carbon may be contained in the aforementioned amounts within the metal lattice such that all or substantially all of the carbon is incorporated into the metal (or other material) lattice, and there are substantially or no carbon aggregates and / or agglomerates at the grain boundaries / lattice surfaces. Furthermore, carbon is preferably present / located at interstitial sites within the lattice.

[0118] Figure 7 illustrates a coating process (Figure 700). This figure relates to a metal substrate subjected to plasma torch spraying of a covetic material, which subsequently produces a composite carbon coating. The metal substrate may include aluminum, copper, iron, nickel, titanium, tantalum, tungsten, chromium, molybdenum, cobalt, manganese, niobium, and their alloys (e.g., various high-nickel alloys as described above). [)] or any one or more of other bulk metallic materials. Covetic materials may include one or more of carbon, graphene, nano-onions, carbon nanotubes (CNTs), carbide implant materials, etc.

[0119] Plasma torch spraying is used to coat input materials with deposited materials and can be operated using pulsed energy. As shown, the deposited material (such as by layer-by-layer sputtering) can be any one or more of carbon, metals (such as those listed above), and / or oxides or nitrides.

[0120] Using the aforementioned torch presents several advantages. The most significant of these advantages is the scalability and versatility of the process, enabling the formulation of unique, stable metal-carbon composites in various configurations / architectures. These configurations / architectures range from fully dense thin-film coatings to thick strips or particles subsequently remelted and cast / shaped into engineered metal alloy components. Each of these materials in the aforementioned range exhibits unexpectedly good (and desired) enhanced mechanical, thermal, and electrical properties compared to existing parent metal alloy formulations. Furthermore, the tunability of the concentration and distribution of covalently bonded 2D graphene in the metal alloy matrix above the thermodynamic dissolution threshold and the layer-by-layer formation in a non-equilibrium plasma environment enables a new class of composite materials that can be engineered for specific applications and / or specific property requirements. Moreover, this is achieved at a significantly lower cost compared to other technologies.

[0121] The enhanced mechanical, thermal, and electrical properties can be applied to applications that heavily utilize copper and aluminum alloys. Examples include (but are not limited to): electrical conductors and high-voltage power transmission cables, microelectronic thermal management and heat exchangers, and many applications using thin-film conductors, such as batteries, fuel cells, and photovoltaics. Specifically, the combination of microwave plasma torch processes with the production of carbon-metal alloys significantly saves energy and improves thermal efficiency during manufacturing, while reducing electrical losses in the final application performance.

[0122] The aforementioned plasma spraying technology only describes one type of method for manufacturing covetic materials. Another type involves spraying carbon particles onto small molten metal particles. This type and its various aspects are shown and discussed with reference to Figures 8A-B, 9, 10, 11, 12, 13, and 14, as well as the discussion in the figures herein.

[0123] Figures 8A-B are schematic diagrams depicting a plasma spraying process 800 for spraying carbon particles onto small molten particles. Alternatively, one or more variations of the plasma spraying process 800 (or any form thereof) may be implemented within the framework and functionality of the embodiments described herein. The plasma spraying process 800 or any form thereof can be implemented in any environment.

[0124] The plasma spraying technology shown is used in various coating processes in which heated materials are sprayed onto a surface. The raw materials (such as coating precursors) are heated by electrical means (such as plasma or electric arc) and / or chemical means (such as via a combustion flame). Depending on the process and raw materials, this type of plasma spraying technology can provide coatings with thicknesses ranging from about 20 µm to about 3 mm. Coatings can be applied to large areas at high deposition rates. Using the above technology, the deposition rate is significantly higher than that achievable through conventional coating processes such as electroplating or physical and chemical vapor deposition.

[0125] In addition to (or alternative to) the exemplary materials described above, coating materials suitable for plasma spraying include metals, alloys, ceramics, plastics, and composite materials. These coating materials are fed into a spray torch in powder or wire form, then heated to a molten or semi-molten state and accelerated toward the substrate in the form of micron-sized particles. Combustion or arc discharge can be used as the energy source for plasma spraying. The resulting coating is formed by the accumulation of many layers of sprayed particles. In many applications, the surface of the substrate does not experience significant temperature rise, thus facilitating the coating of many substances, including most flammable materials.

[0126] Figure 9 is a scanning electron microscope image 900 illustrating the effect of spraying carbon particles (such as those with a particle size of 20 nm to 40 µm) onto small molten metal particles. The carbon particles sprayed onto the small molten metal particles can be used for a variety of specialized applications. For example, plasma aluminum-graphite composites can be specifically designed to provide coatings for turbine engines. Alternatives include the use of aluminum and titanium alloys. The growth rate of the plasma-sprayed coating material is parabolic. The plasma-sprayed coating material deposits within a short time period, and this deposition is largely independent of temperature. To prepare the material surface, some processes include preheating the material. In some embodiments, sandblasting is also used to prepare the metal surface. In some embodiments, portions of the particles sprayed onto the surface remain heated enough to form covetic bonds at the substrate surface. In other cases, the small molten particles are at temperatures sufficient for metal-metal bond formation.

[0127] Compared to conventional torches, the microwave plasma torch technology disclosed herein can produce improved materials. Specifically, the inherent power control limitations and other configuration constraints of conventional plasma torches limit their ability to independently control the input materials and other conditions required for carbon production, which are effective in producing covetic materials exhibiting sufficient quality and homogeneity.

[0128] Figure 10 shows a graph depicting the graphene growth temperature profile Table 1000 and a binary phase diagram. Alternatively, one or more variations of the graphene growth temperature profile Table 1000 or any of its forms can be implemented within the framework and functionality of the embodiments described herein. The graphene growth temperature profile Table 1000 or any of its forms can be implemented in any environment. The figure also shows a binary phase diagram, where the x-axis represents the carbon concentration in the selected metal (such as copper, as shown) as an atomic percentage. The temperatures in the temperature profiles of this figure are also shown in the phase diagram. Various metals (such as silver, tin, etc.) can be used. In some cases, alloys are formed.

[0129] The general idea behind the growth of single-layer graphene (SLG) or few-layer graphene (FLG) on molten metal is to dissolve carbon atoms in a transition metal melt at a certain temperature, and then allow the dissolved carbon to precipitate out at a lower temperature (meaning to produce a solid from the solution).

[0130] The schematic diagram illustrates the growth of graphene from molten nickel by, for example, the following steps: (1) melting nickel while in contact with graphite (as a carbon source); (2) dissolving carbon in the melt at a high temperature; and (3) lowering the temperature to grow graphene.

[0131] As described, based on the metal-carbon binary phase transition, maintaining contact between the melt and the carbon source at a given temperature will cause the carbon atoms in the melt to dissolve and become saturated. As the temperature decreases, the solubility of carbon in the molten metal will decrease, and excess carbon will precipitate at the top of the melt.

[0132] Figure 11 is a cross-sectional view of a (conventional) plasma flame apparatus 1100. This figure is presented to distinguish the use of conventional plasma flame apparatus from the use of the microwave plasma torch disclosed herein. Specifically, while conventional plasma flame apparatus can produce diamond or diamond-like materials on metal surfaces, this process requires a significant amount of time for the dissolution and diffusion of carbon, resulting in the final material depositing onto the metal surface. During the production of the metal-carbon composite material disclosed herein using the currently disclosed embodiments, the desired graphene grows and locks into the gaps between metal or metal-containing composite layers (or within lattice or matrix sites). However, this requires high-rate temperature control. Unfortunately, conventional plasma torches do not provide sufficient control over the temperature and other conditions required to reduce the size of interstitial carbon structures to the nanometer scale (as may be desired for achieving the covetic material described herein).

[0133] In contrast, the pulsed microwave reactor (as described in relation to the previously disclosed embodiments) and the corresponding process are shown and described in Figure 12 to provide sufficiently detailed control over the temperature and other conditions required to reduce the size of interstitial carbon structures to the nanoscale.

[0134] Figure 12 illustrates a pulsed microwave process flow 1200 used when “growing” graphene (referring to the layer-by-layer deposition or application of graphene onto a substantially flat exposed surface of molten metal particles). Alternatively, one or more variations of the pulsed microwave process flow 1200 or any of its forms may be implemented within the architectural and functional context of the embodiments described herein. The pulsed microwave process flow 1200 or any of its forms may be implemented in any environment.

[0135] When the pulsed microwave process flow 1200 shown is used, graphene is grown onto small molten particles. This is accomplished through interactions occurring within the pulsed microwave reactor around the inlet 1204 (where metal powder and carrier gas are introduced into the reactor chamber). In addition to the inlet 1204, process gas ports 1202 and additional ports (such as additional ports 12031 and 12032) are provided at different heights on one side of the reactor apparatus. A waveguide extends at least a distance from the location of the process gas port 1202 on one side of the reactor to the location of the inlet 1204 on the other side of the reactor. Details of how the ports are fabricated and used to introduce and continuously supply material into this reactor for the growth of graphene onto small molten particles are further disclosed below. More specifically, certain components of the reactor of Figure 12 are shown and described with reference to Figure 13.

[0136] Figure 13 is a perspective view of a conventional pulsed microwave plasma spraying waveguide device 1300 for growing graphene onto small molten particles. Alternatively, the pulsed microwave plasma spraying waveguide device 1300 or any of its variations may be implemented within the architectural and functional context of the embodiments described herein. The pulsed microwave plasma spraying waveguide device 1300 or any of its variations can be implemented in any environment.

[0137] In this embodiment, a microwave delivery component and a pulsed power supply are integrated to form a "surfaguide" (or similar) gas reactor. As shown, the combination of these components is configured to facilitate the growth of graphene onto small molten particles using a microwave plasma torch.

[0138] An alternative approach is to perform microwelding using a tungsten inert gas (TIG) plasma source to partially or completely melt the metal. This type of microwelding technique is illustrated and described in Figure 14.

[0139] Figure 14 is a schematic depiction of a microwelding technique 1400 for growing graphene onto small molten particles. Alternatively, microwelding technique 1400 or any of its variations may be implemented within the architectural and functional context of the embodiments described herein. Microwelding technique 1400 or any of its variations can be implemented in any environment.

[0140] Low-power, low-flow TIG welding power supplies and control units with customized plasma containment sections can be effectively used to heat all types of metal particles. As shown, when the exhaust plume is inserted into the surface wave plasma gas dissociation tube, the exhaust plume allows for sufficiently high temperatures to grow graphene. This growth mode, involving the control of plasma radicals composed of hydrocarbons and other additive gases formed under non-equilibrium conditions, provides numerous tuning opportunities that can be utilized by many different configurations of microwave plasma spraying equipment. Figures 15, 18A1, 18A2, 18B, 18C, and 18D, as well as other figures and corresponding written descriptions, illustrate exemplary configurations of plasma spraying equipment.

[0141] Figure 15 is a schematic depiction of a plasma spraying apparatus in coaxial configuration 1500. Alternatively, coaxial configuration 1500 or any of its variations may be implemented within the architectural and functional context of the embodiments disclosed herein. Coaxial configuration 1500 or any of its variations can be implemented in any environment.

[0142] In the coaxial implementation, microwave energy delivery is achieved via a TEM wave fed into the antenna, where the outer portion of the coaxial component is a quartz tube, and the outer surface of the quartz tube contains flowing powdered metal particles. In this example, the gas fed into the central region is a hydrocarbon gas such as methane, which absorbs microwave radiation in the central region. The powder is heated by microwave energy escaping from the central region and external induction heating, causing the metal powder (in particle form) to melt near the tilted portion or tip of the reactor chamber shown. When CH4 decomposes (to its constituent substances, carbon, hydrogen, and / or their derivatives), carbon radicals nucleate on the surface of the molten metal droplets via the energy of plasma radicals. Tuning the microwave duty cycle, the induction heating, and the plasma characteristics helps maintain different temperatures between the melt and the plasma decomposition / ionization region. Furthermore, the non-equilibrium temperature allows (promotes) the internal lattice placement of graphene / carbon, and rapid quenching creates conditions favorable for the growth of other covetic materials.

[0143] Figure 16 is a schematic depiction of a plasma spraying apparatus 1600 illustrating the evolution of a material processed under a series of non-equilibrium energy conditions. Alternatively, one or more variations of the plasma spraying apparatus 1600 (or any form thereof) may be implemented within the architectural and functional context of the embodiments disclosed herein. The plasma spraying apparatus 1600 or any form thereof can be implemented in any environment.

[0144] This figure depicts the evolution of the material as it passes through the device. Specifically, it depicts regions where different gradual changes occur, such that graphene grows onto small molten metal particles in the region near the tip. This material is then deposited onto a substrate.

[0145] Figure 17 illustrates a surface wave plasma system 1700 for growing graphene onto molten particles. Alternatively, the surface wave plasma system 1700, or any variant thereof, may be implemented within the architectural and functional context of the embodiments disclosed herein. The plasma system 1700, or any variant thereof, can be implemented in any environment.

[0146] In the configuration shown, a supply gas is fed into the central region of the device. In this example, a hydrocarbon gas such as methane is used. The hydrocarbon gas absorbs microwave radiation, which provides a heat source for heating the metal powder. Therefore, the metal powder is heated to melt and become molten near the tip using both: (1) microwave energy escaping from the central region; and (2) external induction heating. When the hydrocarbon gas decomposes, carbon radicals nucleate on the surface of the molten metal droplets via the energy of plasma radicals.

[0147] Figure 18A1 depicts the axial field configuration 1810 of a plasma spraying torch. The formation of covetic materials has been discussed using several different devices and corresponding processes. Any of the aforementioned devices and processes can be tuned to achieve specific conditions for forming covetic materials. In the specific axial field configuration shown, the process includes generating an electric field 1804 between electrodes to produce a current through a molten metallic and carbon material. Specifically, and as shown, the plasma torch in this particular configuration has an externally controlled field in which molten particles form a plasma, which then becomes the primary electrode. The electrode on the other side of the field is formed by the growth plate 1803 shown. The covetic material is accelerated through the acceleration region 1821 and then deposited onto the surface. The resulting alloy and covetic material continue to be deposited onto the growth plate and / or the previously deposited material in the collision region 1823. This deposition technique produces a material with homogeneous and high carbon loading.

[0148] The input materials can be selected and modified to achieve materials exhibiting specific properties. For example, as shown, the input of the plasma spraying torch may include various input gases 1812 and input metal and / or carbon particles 1818. These inputs can be introduced into one or more input ports 1862. In some cases, the input metal and / or carbon particles are entrained within the flow of input gas 1812. Furthermore, the growth plate can change its size and composition during the ongoing deposition process. For example, as shown, the growth plate 1803 may initially be a substrate 1816 on which a thermally covetic material from the torch stream is deposited, which at least partially melts the substrate during the deposition of the covetic material. The deposited thermally covetic material cools from a molten or partially molten state to form a quenched layer.

[0149] In this way, any number of layers can be formed. The temperature at or near the substrate and / or the top layer can be controlled so that when the next layer of material is deposited on the molten metal of the previously deposited layer, the newly deposited layer grows laterally to produce a monolayer of graphene on the surface of this molten metal. This mechanism differs from other techniques, at least in that, compared to the conventional metal melting method 103 in which carbon precipitates from the molten metal slurry, the application of the plasma spraying torch method 104 disclosed herein results in quenching within a short period of time, leaving insufficient time for carbon to precipitate from the matrix. Therefore, the covetic bonds remain intact throughout the layer. Moments later, after quenching to form a solid metal and well-dispersed carbon, another layer is sprayed on top, and so on, thereby forming a monolayer of graphene. These layers grow, trap, and rapidly quench to produce a truly covetic material with extremely high carbon loading within the matrix. As an example, when using the conventional metal melting method 103 (see Figure 1A), a carbon loading of 6% carbon metal can be achieved. In contrast, when using the plasma spraying torch method 104 (see Figure 1A), a carbon loading of 60% can be easily achieved. In some cases, strict control over the input and process parameters of the plasma spraying torch and its environment allows for a carbon loading in the resulting material that is close to or even reaches 90%.

[0150] Experimental results using plasma spraying torches have demonstrated that highly uniform covetic layers with high loading can be formed using at least two rapid quenching (such as "sputtering") methods. The first method introduces carbon particles to cover metal particles (e.g., in plasma), and then sprays the resulting thermal mixture onto a substrate at a much lower temperature. The second method generates graphene in plasma and then introduces molten metal to cover the graphene. In both cases, true covetic bonding (referring to a combination of covalent and metal chemistry) occurs while in the plasma plume, and the rapid quenching of the spray is used to trap the mixture within the organometallic lattice.

[0151] As shown in Figure 18A2, the depth or thickness of the quenched layer 1824 can be made thicker or thinner by controlling the distance between the plasma flame 1814 and the substrate and / or by controlling the temperature at the substrate 1816 (such as being higher or lower than the ambient temperature) and / or by controlling the pressure inside and around the reactor.

[0152] Figure 18B depicts a radial field configuration 1820 of a plasma spraying torch. In this configuration, molten particles form a plasma within the torch, where the plasma becomes the primary electrode. Other electrodes are formed from one side of the inner wall.

[0153] The configurations described in Figures 18A1, 18A2, and 18B are merely examples. Other configurations involving different input materials and different input port configurations are possible without departing from the generality of the plasma spraying torch disclosed herein. Furthermore, different configurations involving different input materials and different input port configurations can achieve the same expected results. For example, two different configurations tuned to achieve the same resulting material are shown and described with reference to Figures 18C and 18D. Specifically, the exemplary configurations in Figures 18C and 18D can be used to deposit ceramic film materials onto carbon-containing particles (such as graphene-containing particles) using a plasma spraying torch.

[0154] In fact, thin film deposition of carbon-containing materials (such as via atmospheric pressure chemical vapor deposition (APECVD) and / or other variations of chemical vapor deposition (CVD)) has entered many fields of materials processing. Various composite materials and coatings involving such carbon-containing materials can exhibit improved physical properties (such as strength, corrosion resistance, etc.). The molecular-level configuration within carbon-containing materials, along with the morphological characteristics of various 2D and 3D carbons, contributes to these improved physical properties in composite materials and coatings. In some cases, the use of 2D and 3D carbons in composite materials and coatings significantly improves the high-temperature resistance of the resulting carbon-containing materials; however, in other cases, these temperatures rise to above ~2100°C, high enough to burn the 2D and 3D carbons themselves. Unfortunately, the destruction of 2D and 3D carbons consequently destroys the initial benefits derived from carbon in the composite material or coating. Therefore, deposition techniques (such as plasma torch configurations) are needed to produce composite materials or coatings unaffected by temperatures above the carbon combustion temperature.

[0155] Figure 18C depicts this configuration, but is only a non-limiting example. By adjusting the input and various reactor conditions, graphene-containing materials can be coated with an endothermic layer of organically modified silicon (ORMOSIL). The deposition of ORMOSIL ceramic materials onto graphene-containing materials can be achieved through several methods, including atmospheric, reactive plasma-enhanced chemical vapor deposition processes using silicon-containing precursors 1841 (such as hexamethyldisiloxane) and reactive gases such as oxygen. This particular mixture of silicon-containing precursors and oxygen is reactive within the plasma. Molecular dissociation occurring within the plasma flame leads to the deposition of silicon oxide onto surfaces such as the aforementioned growth plate 1803. Therefore, reactor conditions are controlled so that the organically modified silicon ceramic is deposited onto its surface as carbon-containing particles form within the reactor. Controlling in-reactor growth and deposition (such as by controlling the APECVD process) results in the formation of a thin quartz coating around carbon-containing particles, which are then deposited onto the substrate. This thin quartz coating acts as a flame-retardant layer to prevent the carbon-containing particles from burning at high temperatures.

[0156] Figure 18D depicts an alternative configuration, which is only a non-limiting example. As shown, metallic and / or carbon-containing materials are fed into the reactor. The microwave energy 1822 is controlled to at least reach the temperature required to dissociate the carbon-containing material (such as T(c-dis) in Figure 10). A silicon-containing precursor 1841 (such as HMDSO, HMDSN, etc.) is introduced into the plasma flame, and the temperature in the plasma afterglow is lowered. Due to the temperature reduction, carbon particles begin to form and become coated with silicon oxide. The silicon oxide-coated carbon particles are then deposited onto a substrate.

[0157] In one embodiment, a thin layer of these 3D materials, approximately 10 nm thick, can be deposited onto a substrate that will not burn or ignite even at 1200°C. This is because the original carbon (such as graphene) is crystalline, thus it is not an amorphous material. Rather, the original carbon has been transformed into a state in which it can no longer be burned.

[0158] In one application, the aforementioned plasma spraying torch technology can be used to produce novel non-eutectic solders. Alternatively, in another application, the plasma spraying torch can directly spray a material coating onto a substrate to prevent oxidation of the underlying material.

[0159] Besides forming materials that do not burn even at 1200°C under atmospheric pressure, placing quartz around materials usually produces great application advantages.

[0160] Besides organically modified silicon, other organic substances can also be used to coat carbon particles or carbon layers. The properties of the coating can be controlled. As an example, the pores on the surface of the sprayed material can be tuned to be hydraulically smooth.

[0161] Plasma spraying torches can be used to form endothermic, glass-coated, non-flammable graphene composed of graphene and silicon, wherein the silicon coating enables the graphene to withstand temperatures above 1600°C. This endothermic, glass-coated, non-flammable graphene absorbs infrared energy.

[0162] A specific method for producing an organically modified silicon coating includes the following steps (e.g.): (1) introducing a silicon-containing precursor into a plasma spraying torch apparatus; (2) combining the silicon-containing precursor with a carrier gas having carbon particles entrained in the precursor gas; and (3) coating the carbon particles with silicon.

[0163] The properties of flame-retardant and infrared-shielding materials produced by the plasma-spraying torch configurations of Figure 18C and / or Figure 18D can be tuned, at least in part, by controlling the time-temperature path within the reactor. More generally, the properties of materials produced by the plasma-spraying torch configurations of Figures 18A1, 18A2, 18B, 18C, or 18D can be tuned, at least in part, by controlling (e.g., pulsed) microwave energy within the reactor.

[0164] Figure 19 is a table 1900 depicting the energy versus time during pulse on and off. More specifically, the figure shows a complete time cycle from time T = 0 to 50 microseconds, during which the microwave is continuously turned on, and then the remainder of the cycle depicts the time during which the microwave is turned off. The plotted curves depict (1) the change in density and (2) the change in temperature during the cycle. At time T = 0, the temperature is at its lowest point (as depicted at the origin of the figure). The temperature rises rapidly and then falls, during which time the plasma density reaches a relatively stable value. When the microwave is turned off at time T = 50 microseconds, both the plasma density and the temporary electron temperature drop rapidly. The pulse time and duty cycle can be controlled to achieve specific densities and temperatures at any given time.

[0165] Figure 20A1 depicts an image showing the organometallic bonding that occurs when carbon and copper are combined using a plasma spraying torch. As shown, carbon 2052 is deeply embedded in copper 2054. As commonly understood and mentioned herein, organometallic chemistry refers to the study of organometallic compounds, compounds in which at least one chemical bond exists between the carbon atoms of an organic molecule and a metal (including alkali metals, alkaline earth metals, and transition metals, and sometimes extended to include metals such as boron, silicon, and tin). In addition to bonding with organic radical segments or molecules, bonding with "inorganic" carbon (such as carbon monoxide (carbonyl metal), cyanide, or carbides) is generally also considered organometallic. The discussion of organometallic compounds may include related compounds such as transition metal hydrides and metal phosphine complexes, but strictly speaking, they are not necessarily organometallic.

[0166] In organometallic chemistry, organocopper compounds contain carbon-copper chemical bonds and can possess unique physical properties, synthesis, and reactivity. The structures and reactivity of organocopper compounds can vary widely, but there are still some restrictions on the oxidation state of copper(I), such as representing it as Cu+. As a d10 metal center, it is associated with Ni(0), but due to its higher oxidation state, it participates in fewer π-backbondings. Organic derivatives of Cu(II) and Cu(III) can be referred to as intermediates, but they are rarely isolated or even observed. Geometrically, copper(I) adopts a symmetrical structure consistent with its spherical electron shell. Typically, one of three coherent geometries can be used: linear 2-coordinate, trigonal 3-coordinate, and tetrahedral 4-coordinate. Organocopper compounds form complexes with various soft ligands, such as alkylphosphine (R3P), thioethers (R2S), and cyanides (CN-).

[0167] Using any one or more of the techniques described above, the carbon depicted in Figures 20A1 and 20A2 can be chemically bonded to copper, rather than simply juxtaposed with copper to adhere via Van der Waals forces (such as distance-dependent interactions between atoms or molecules). Unlike ionic or covalent bonds, Van der Waals forces are not generated by chemical electronic bonds; they are relatively weak and therefore more susceptible to interference. Furthermore, Van der Waals forces dissipate rapidly at longer distances between interacting molecules. Instead, organometallic bonds between the metal and carbon are desired.

[0168] Figure 20A2 depicts a hierarchical composition of a substance applied to a substrate material and shows images of three material property regions. The bulk metal region 2066 is the first material property region of the three material property regions. As shown, the first material property region comprises a metal in a first crystal form having significant metallic bonds between the metal atoms present in the first material property region. This first material property region is substantially adjacent to a second material property region that at least partially overlaps with the first material property region. The covetic material region 2064 comprises at least some carbon atoms in a second crystal form having at least some nonpolar covalent bonds located between some carbon atoms present in the second material property region and metal atoms present in the first material property region. The top surface region 2062 is a third material property region that at least partially overlaps with the second material property region. This top surface region comprises additional carbon atoms oriented in a third crystal form. The third crystal form is characterized by at least some nonpolar covalent bonds between individual carbon atoms in the additional carbon atoms present in the third material property region. In various embodiments, some metal atoms and some carbon atoms may be present in any of these regions. However, this embodiment is characterized by a higher metal content region 2074 adjacent to the body metal region 2066. In various embodiments, some carbon atoms and some metal atoms may be present in any of these regions. However, this embodiment is characterized by a higher carbon content region 2072 adjacent to the top surface region 2062.

[0169] Figure 20B is a material evolution table 20B00 depicting several layering configurations that occur when carbon is added to the bulk aluminum. In these embodiments, the material is sprayed onto an existing carbon-rich covetic substrate or carbide layer to create carbon-to-carbon bonding via carbon sintering and / or molten metal encapsulation, thereby creating an adhesion to form a composite film. Material evolution table 20B00 is only one example of a composite material (silicon carbide) sprayed onto the aluminum bulk material. This process can be tuned to produce a covetic or covetic sample film deposited onto the bulk material. The resulting material can then be coated to create a functionalized top layer. One possible configuration of the apparatus for spraying the composite material onto the substrate is shown in Figure 21A.

[0170] Figure 21A depicts an apparatus for spraying a molten mixture of materials onto a substrate. The figure illustrates a microwave reactor comprising multiple zones within a storage container. Pulsed microwave energy is delivered into the storage container. A hydrocarbon process gas 605 is supplied via an inlet port. The microwave energy heats the process gas to a sufficiently high temperature to form a plasma. The expansion of the material within the storage container generates a plasma plume. Continuous addition of material to the storage container, combined with the aforementioned expansion, creates a torch effect in and around the plume. Due to the high temperatures within and around the plasma plume, carbon and hydrogen dissociate, forming several different hydrocarbons (such as CH3, CH2). As the temperature continues to rise (as shown in the first zone 2104), all or almost all carbon atoms dissociate from hydrogen. Using any known technique (such as a gas-solid separator), the hydrogen-containing material is separated from the solid carbon material.

[0171] At the interface between the first region 2104 and the second region 2106 of the storage container, molten metal, molten metal composite, molten ceramic-metal, metal matrix, or any kind of metal mixture is introduced into the storage container (as shown) via a second inlet. The location of the second inlet is selected based on the size of the plasma plume and / or the temperature of the molten metal at the inlet point into the storage container. More specifically, molten metal 2108 is introduced into the reactor at the location where the molten metal is mixed with the carbonaceous material. As the mixture flows through the storage container (e.g., at a high rate), the mixture cools to a lower temperature. The flowing mixture exits the storage container at a high rate, causing the mixture of carbon and molten metal to be ejected from the outlet 2110. The mixture is deposited (e.g., by spraying a coating material 2112) onto the target substrate 2116. Various mechanisms for controlling the uniformity of the coating material 2112 and / or the resulting deposited material 2114 are shown and discussed with respect to Figures 23A to 23D.

[0172] The temperature in the second region is low enough that at least some of the carbon precipitates from the mixture. However, most of the dissociated carbon remains mixed with the molten metal. When the molten metal mixed with carbon reaches the target substrate 2116, it cools into a solid. During the transformation from a molten mixture to a solid deposit, carbon is trapped between the metal and carbon layers. At certain temperatures, carbon forms nonpolar covalent bonds with the metal, thus producing a covetic material. Due to the increased cohesive forces (such as nonpolar covalent bonds) between the metal matrix and carbon, this covetic material exhibits a range of mechanical, thermal, electrical, and tribological properties.

[0173] This type of covetic material is the result of using pulsed microwave energy to control the energy distribution of the material components in the first and second regions of a reactor. More specifically, the energy distribution of the material components in the first and second regions of the reactor can be controlled partly by pulsed microwaves and partly by pre-melting the metal particles in the external environment of the reactor chamber (e.g., to introduce fully molten or partially molten metal into the reactor chamber). Any known technique can be used alone or in combination to melt the metal particles. In this way, the degree of fully molten or partially molten particles and / or mixing can be controlled.

[0174] Figure 21B depicts a method for spraying covetic material onto a substrate. This method can be used in conjunction with the apparatus shown in Figure 21A. As shown, the method is performed using a microwave reactor having an inlet for process gas, an inlet for molten metal, and an outlet. Prior to operation, the microwave reactor is configured to have an inlet for hydrocarbon process gas, an inlet for molten metal, and an outlet (operation 21B02). In operation 21B10, the inlet is used to introduce the hydrocarbon process gas into the first region of the reactor. Using microwave energy, the temperature in the first region of the reactor rises, causing the hydrocarbon process gas to dissociate into carbon and hydrogen substances before contacting the molten metal. The other inlet is used to introduce the molten metal into the second region of the reactor (operation 21B20). The high temperature in the second region is maintained until the dissociated carbon mixes with the molten metal (operation 21B30). The aforementioned plume is used to move the mixture to the third region of the reactor (operation 21B40). Moving the mixture away from the microwave energy source has the effect of lowering its temperature until at least some of the carbon in the mixture condenses out (operation 21B50). However, even with the temperature reduction, the plasma torch effect still allows the mixture to be moved through the outlet at a high rate (operation 21B60). Thus, the molten mixture is sprayed onto the substrate (operation 21B70).

[0175] Figure 21C is a schematic diagram depicting a plasma spraying process for coating films. As shown, carbon radicals, polycyclic aromatic hydrocarbons, graphene sheets, and metal particles are mixed at high temperatures in a plasma reactor (such as the first region 2104 shown). Nucleation occurs at these high temperatures, and growth and aggregation begin as the temperature decreases within the reactor (such as the second region 2106 shown). A possible growth mechanism is depicted using submicron-sized aluminum particles coated with few layers of graphene. These submicron-sized aluminum particles can be held together using a combination of metallic bonds, nonpolar covalent bonds, and covetic bonds. More specifically, and as shown at the 2 nm scale, carbon atoms are bonded to aluminum atoms. The carbon atoms are organized into coherent graphene planes located within the aluminum matrix, preferably interlaced between the basal planes of the aluminum matrix. The foregoing discussion regarding aluminum is merely illustrative. Other metals may be used. In fact, coherent graphene planes can be located not only in face-centered cubic (FCC) metal lattices (preferably between basal planes), but also in body-centered cubic (BCC) metal lattices or hexagonal close-packed (HCC) metal lattices.

[0176] The coated particles are then sintered to form particles with a diameter of approximately 100 µm. These semi-molten particles are then accelerated through the reactor and collide with the substrate (e.g., during the first pass) or with the previously deposited impact particle layer (e.g., during the second or Nth pass).

[0177] Figure 22A depicts an apparatus for encapsulating carbon particles with molten metal. The configuration of the apparatus in Figure 22A differs from that in Figure 21A, at least in that the introduction of molten metal is controlled using melting device 2209. When the molten metal is introduced into the reactor, the molten metal is controlled to produce molten metal encapsulating the carbon particles.

[0178] Figure 22B depicts a method for encapsulating carbon particles with molten metal. Prior to operation, the microwave reactor is configured with an inlet for hydrocarbon process gases, an inlet for molten metal, and an outlet (operation 22B02). In operation 22B10, the inlet is used to introduce the hydrocarbon process gases into a first region of the reactor. This method differs from that of Figure 21B, at least in that, in operation 22B30, the temperature in different regions of the reactor is maintained, allowing some carbon particles to form from dissociated carbon. The aforementioned plume is used to move the mixture to a third region of the reactor (operation 22B40). In operation 22B50, at least some of these carbon particles are encapsulated by molten metal. Bonds are formed between the constituent atoms of the carbon particles and the atoms of the molten metal. In operation 21B60, the metal-encapsulated carbon particles move through the outlet, further reducing the temperature. As the metal-encapsulated particles deposit onto a substrate (operation 21B70), further bonds are formed between the metal-encapsulated carbon and the metal of the substrate.

[0179] Figures 23A, 23B, 23C and 23D depict exemplary deposition techniques according to some embodiments.

[0180] As shown in Figure 23A, the deposited material has a curved shape, characterized by a higher middle region and a lower end region. In some cases, this is the desired shape for a small amount of deposited material. In other cases, it is desirable to spray the deposited material onto a larger area. This can be achieved by moving the substrate relative to the spray or by moving the spray relative to the substrate. Figure 23B depicts a flexible substrate 2310 arranged on a feed reel. The flexible substrate can be pulled onto and around a take-up reel. Thus, in the configuration of Figure 23B, the spray uniformly deposits covetic material onto the moving substrate. When the relative movement between the sprayed material 2112 and the substrate is controlled, the resulting deposited material has a uniform thickness.

[0181] In some cases, it is desirable to have a non-uniform but uniform pattern on the surface of the deposited material. In such cases, the substrate can be moved progressively through a series of discrete positions to form the pattern shown in Figure 23C. Alternatively, a slotted antenna can be disposed between the sprayed material 2112 and the substrate. The slotted antenna functions by uniformly distributing the spray across the lateral distance of the slotted antenna. Using this slotted antenna, a single point of the sprayed material 2112 can have substantially the thickness and surface uniformity shown in Figure 23D.

[0182] Figures 24A and 24B illustrate conventional techniques for depositing materials onto a substrate. As shown in Figure 24A, carbon aggregates are held together using a binder (such as a polymer). This results in weaker bonding at the interface between the carbon aggregates and the substrate. Figure 24B illustrates the application of a binder to coat carbon material onto a substrate. Conventional deposition using a binder suffers from the adverse effects of peeling. Furthermore, even when the substrate surface undergoes mechanical pretreatment and / or pretreatment via the deposition of a binder material, the interaction between the substrate and the carbon aggregates remains weak.

[0183] As previously mentioned, coatings deposited onto a substrate using adhesives and / or coating techniques (such as those shown and described with respect to Figures 24A and 24B) suffer from adverse effects such as peeling, low strength characteristics, and other undesirable mechanical properties. Improvements based on plasma spraying technology are shown and discussed in Figures 25A and 25B.

[0184] Figures 25A and 25B illustrate exemplary deposition techniques for generating nonpolar covalent bonds on the surface of a substrate according to some embodiments. Specifically, as shown, when using the techniques disclosed herein, a covetic material is formed by nonpolar covalent bonds between carbon and the substrate. Thus, no binder is needed or used. Furthermore, many of the nonpolar bonds formed at the interface between the substrate and the covetic material are strong covalent bonds. In one particular case, when the substrate is aluminum, nonpolar covalent bonds are formed between atoms in the face-centered cubic structure of aluminum and carbon atoms in the hexagonal structure. Figure 25B depicts a schematic diagram of the interfacial bonding.

[0185] Figures 26A, 26B, 26C, and 26D present schematic diagrams illustrating how nonpolar covalent bonds are formed between sites in the square shape of the face-centered cubic structure of aluminum and sites in the hexagonal shape that appear in certain crystal structures of carbon.

[0186] Figure 26A is an orthographic view showing the square shape of the face-centered cubic structure of aluminum. Figure 26B is an orthographic view showing the hexagonal shape that appears in some crystal structures of aluminum.

[0187] Figure 26C depicts a possible superposition of hexagonal shapes appearing in certain crystal structures of carbon on top of a square shape in the face-centered cubic structure of aluminum. Figure 26D depicts nonpolar covalent bonds formed at certain sites. The example of the face-centered cubic structure of aluminum is only one example. Other metals with other crystal structures are possible. The unexpected properties exhibited by some embodiments are assumed to be caused by the nonpolar covalent bonding between carbon atoms and metal atoms being sufficient / effective to "trap" all or substantially all (e.g., at least 90%, at least 95%, at least 98%, at least 99%, etc.) of "free" electrons normally present in compounds exhibiting metallic bonding, thus altering the properties usually associated with the presence of "free" electrons in metals and metal-containing compounds. For example, some embodiments may be characterized by the fact that the surface of the innovative material composition does not actually have "free" electrons, thus exhibiting reduced thermal conductivity and / or electrical conductivity. Furthermore, for embodiments that do not actually have "free" electrons, the surface of the innovative composition does not oxidize when exposed to ambient air.

[0188] Figure 26E shows an example of the layered covetic material 26E00, in which a graphene-like structure is sandwiched between layers of metal material. The lower layer of the metal material is a substrate layer. The top layer of the metal material is formed from quenched material that was previously melted while in a reactor. Due to the formation of metal-metal bonds between the two metal layers, the graphene-like structure sandwiched between the metal material layers is trapped between the two metal layers. In addition to the metal bonds, other bonds are also formed to surround the graphene-like material between the metal layers. In some locations, defects exist in the carbon lattice. Various types of bonds form between or near these defects.

[0189] Any or all of the aforementioned techniques for forming covetic materials can be used in many applications involving many different types of substrates. Furthermore, the relative movement between the spray and the substrate can be controlled to produce a deposit of any thickness. Any known technique can be used to control the relative movement. For example, the outlet can be moved on a fixed substrate. This can be achieved using a handheld device or a robot-controlled device that moves relative to the fixed substrate. In some cases, the substrate can be subjected to a bias voltage, causing at least some of the material ejected from the outlet to be electrostatically attracted to the surface of the substrate. This is applicable in applications where the substrate is not uniformly flat. Examples of applications where the substrate is not uniformly flat include: (1) forming components in machinery subjected to harsh corrosive conditions; (2) turbine blades; (3) heat exchanger assemblies, many of which will be discussed further below.

[0190] In other cases, the properties of the deposited material (such as thickness, lateral uniformity, etc.) can be enhanced by using various chemical vapor deposition techniques and / or combinations of various chemical vapor deposition techniques. As just one example, the properties or parameters associated with plasma-enhanced chemical vapor deposition techniques known in the art can be controlled to optimize the characteristics of the deposited covetic material layer. As another example, instead of depositing the covetic material onto a surface to form a film or coating, the covetic material can be formed into particles (such as by spraying into a lower temperature environment) and collected in powder form. Various techniques involving the production and use of powdered covetic materials are briefly discussed below. [, powder , ] [, covetic , ] [, Material , ] [, , ]

[0191] In some cases, instead of forming the covetic material as a film or coating on or within a substrate, the covetic material can be delivered in the form of a covetic material powder. This powdered covetic material can be collected upon exiting the reactor, cooled to a temperature below the melting point of the covetic material, and collected in powder form. The powder can then be processed at room temperature (such as storage and transport, dumping, mixing, etc.). The powder can then be remelted and pressed into a molded part or remelted and recoated. As an example, components used in highly corrosive environments can be formed from such powdered covetic materials using injection molding or extrusion. Many devices can be used individually or in combination to form and transport covetic material powders. Illustrative devices are shown and discussed with reference to Figures 27A, 27B1, and 27B2.

[0192] Figure 27A depicts an exemplary apparatus 27A00 for cooling the sprayed material 2112 to produce powdered covetic material 2710 using a cooling zone 2702 when the spray is forced through the outlet 2110 of a microwave reactor. Any one or more cooling techniques in any combination can be used to reduce the temperature of the covetic material in the cooling zone 2702 to below the melting point of the covetic material. The cooling zone 2702 may house one or more devices to induce cooling. For example, and as shown, the collection container 2704 may be fitted with one or more devices to induce a cyclone effect in the collection container, thereby increasing the time for reducing the temperature of the covetic material. In some cases, the cooling time of the covetic material is controlled (e.g., by increasing or decreasing the time) to allow the covetic material to anneal with highly regular bonds. In some cases, controlling the cooling time of the covetic material allows the covetic material to crystallize into a highly regular crystalline structure while still remaining in powder form. In some embodiments, a mechanical drum-stirrer may be installed between the microwave reactor outlet 2110 and the collection container 2704. The drum-stirrer can be cleaned or replaced periodically.

[0193] Alternatively or additionally, and where it is convenient and / or necessary to contain and / or transport powdered covetic materials in a fluid, a fluidized bed apparatus may be used. For example, to avoid the formation of aggregates and / or agglomerates of powder particles, the powdered covetic material may be held (e.g., suspended) in a liquid. In some embodiments, the fluidized bed apparatus may be mounted between the outlet 2110 of the microwave reactor and the collection container 2704. One embodiment of such a fluidized bed apparatus is shown and described with reference to Figures 27B1 and 27B2.

[0194] Figures 27B1 and 27B2 depict an exemplary fluidized bed apparatus 27B00 for cooling and treating powdered covetic materials in fluids.

[0195] As shown, the molten metal and carbon mixture is forced through the reactor outlet and into the top of the fluidized bed 2750. As the molten metal and carbon mixture is forced out of the outlet, it cools by forming particles. The particles are acted upon by downward gravity (as shown, in the downward direction) while simultaneously being driven upward by the process fluid 2754 from the bottom of the fluidized bed. Thus, the particles accelerate toward the bottom of the fluidized bed at a rate of acceleration slower than that of local gravity. The flow dynamics can be partially modulated by the geometry of the fluidized bed. For example, and as shown, a fluidized bed of a certain length can be formed into a conical body 2762, wherein a first end of the conical body has a first dimension D1, and a second end of the conical body has a second dimension D2, wherein D1 > D2. The temperature within each part of the fluidized bed can be controlled in part by a power supply 2752 (as shown) that supplies power to the coils and / or by a heat source 2760 that heats the process fluid 2754 before it enters the bottom of the fluidized bed.

[0196] The pressure, flow rate, and other conditions within and at the interface of a fluidized bed are used to cause the powder and fluid mixture to behave as a fluid. This mixture exhibits many properties and characteristics of fluids, such as the ability to flow freely under gravity and / or the ability to be pumped using fluid handling techniques.

[0197] In the embodiments of Figures 27B1 and 27B2, the fluidized bed has multiple ports positioned at different heights of the conical body. This allows a first powder 27561 in the fluid to flow out at a specific temperature / pressure, while a second powder 27562 in the fluid flows out at a second, different specific temperature / pressure. The flow rate through the multiple ports can be controlled, allowing the collection container to hold any ratio or amount of the first powder 27561 and the second powder 27562 in the fluid. [, form , ] [, covetic , ] [, Materials and Methods , ] [, , ] Table 3 shows some non-limiting examples of methods for forming powdered covetic materials. Illustrative methods name Illustrative method 1 Organometallic materials are produced by dissociating hydrocarbon process gases in a plasma spraying torch based on a microwave reactor. Illustrative method 2 Carbon allotropes are grown on input particles within a microwave reactor. Illustrative method 3 After dissociating alternative process gases in a microwave reactor-based plasma spraying torch, the input material is coated. Table 3 [, , ] [, Illustrative methods , ] [, 1 , ]

[0198] In some embodiments of Method 1, structured carbon (such as carbon allotropes) is formed in a first region of a microwave reactor (e.g., via dissociation of hydrocarbon process gases). In a second region at a lower temperature than the first region, the structured carbon is decorated with metal to form a metallized carbon material (such as an organometallic material). The metallized carbon material is further cooled to a temperature below the melting point of the metal. In some embodiments, the metallized carbon material is initially in the form of metallized carbon particles. The particles are further cooled to form a powder. This powder can be collected and transported to an application facility. The powder containing the metallized carbon material with covetic bonds can be remelted and used with any known technique for forming components from powder. By way of example only, components can be formed from powder using molding followed by remelting, isostatic pressing followed by remelting, hot forging, metal injection molding, laser sintering, etc. [, Illustrative methods , ] [, 2 , ]

[0199] In this method 2, one or more hydrocarbon gases (or in some cases, gases and liquids) are introduced into the system. By way of example only, the gases and / or liquids that may be introduced into the system include methane, ethane, methylacetylene-propane (MAPP), and hexane. In a first region 2104 at a first temperature, carbon atoms dissociate from other atoms (such as from hydrogen). Molten metal 2108 is introduced into the reactor as metal particles. Then, in a second region 2106, the carbon produced in the first region combines with the metal particles. Carbon may grow on the surface of the metal particles and / or within the metal particles. In some cases and under some conditions, carbon growth includes the growth of 2D carbon on or within the metal particles. In other cases and / or under other conditions, carbon growth includes the growth of 3D carbon on or within the metal particles. In any of the aforementioned growth scenarios, the growth may occur to the maximum extent permitted by the crystal lattice. For example, the molten metal may be aluminum with a face-centered cubic (FCC) crystal structure, and the carbon may form a solid solution with a certain concentration of aluminum. In some embodiments, carbon is formed in a solution of metal having a concentration of up to that determined by the metal's properties (such as crystal structure), and then precipitated from the metal-carbon solution to form 2D or 3D carbon on and / or within the metal particles.

[0200] The growth system in this method 2 is carried out under non-equilibrium thermal conditions. Specifically, various thermal conditions are used to control, for example, the following: (1) a first temperature (such as a higher temperature) in the first region required to control the aforementioned dissociation, and (2) a second temperature (such as a lower temperature) in the second region used to control the initial melting of the metal powder and / or the formation and properties of the metal-carbon particles in the second region. The temperatures in these two regions can be controlled independently. Using this method, the sprayed material is a truly covetic material exhibiting truly covetic properties. [, Illustrative methods , ] [, 3 , ]

[0201] In other non-limiting examples, the material and / or coating on the input particles may be generated or deposited from mixtures such as trimethylamine (TMA), trimethylglycine (TMG), and methylacetylene-propane. The particles may be cooled and collected in powder form. Some examples of particles that can be generated from the target material in the first region are phase-controlled carbon, silicon carbide, metal oxides, metal nitrides, or metals. In some cases, the input particles are metals, and a compound film (such as a metal oxide or metal nitride) is coated on the metal input particles; in other cases, the input particles contain compound material, and a metal coating is deposited on the input particles. Some examples of particles that can be generated from the input gas in the first region are carbon allotropes (such as native carbon), silicon, ZnO, AlOx, and NiO.

[0202] In some embodiments, a gas comprising various non-hydrocarbon gases or alcohols is introduced into a first region, and the first region includes a sputtering apparatus and a power supply, wherein the sputtering apparatus is configured to generate various ionic substances from a selected target material. The target material and ionic substances are combined to form multiple particles. The power supply may be an AC, DC, RF, or high-power pulsed magnetron sputtering (HIPIMS) power supply and may be configured to generate various ionic substances from the target material by tuning power, voltage, frequency, repetition rate, and / or other characteristics of the power supply.

[0203] Figure 27C is a schematic diagram depicting a plasma spraying process for producing powdered covetic materials. [, Powder material processing sequence , ] [, , ]

[0204] Figure 27C shows a visual representation of an exemplary powder material processing sequence, from hydrocarbon cracking and particle nucleation (such as the first region 2104 shown) to graphene growth (such as the second region 2106 shown), cooling of semi-molten particles (such as in the cooling region shown), and collection of powdered covetic material (such as in the collection region and into collection container 2704). The mechanisms behind the effectiveness of this exemplary powder material processing sequence will now be briefly discussed.

[0205] In the absence of a metal precursor (whether in organometallic or particulate form), microwave plasma dissociates methane to form carbon radicals (and polycyclic aromatic hydrocarbons / acetylene), which then form few-layer (FL) graphene (or stacked sheet) structures, respectively. However, in the presence of a metal precursor in the plasma region (such as the reactors shown in Figures 21A and 22A), the metal (from organometallic cores or particles) can be used as a seed site for heterogeneous carbon growth (such as carbon in the form of ionized radicals, graphene cores, or polycyclic aromatic hydrocarbons (acetylene)).

[0206] When using metals with low solubility, such as Al or Cu, graphene sheets can be grown onto metal surfaces (e.g., via adsorbed atoms / monomers or as clusters). The characteristics of the growth depend at least in part on the symmetry and minimization of the interfacial free energy at the metal surface. Thus, carbon growth occurs at the metal particles while metal atom re-sputtering events occur at the surface to produce mixed and / or layered metal / carbon structures. As is known in the art, the radius of the metal particles (such as surface curvature) can affect the solubility of carbon in the metal particles. As an example, a smaller radius (such as corresponding to a higher curvature) increases the solubility beyond equilibrium (on a flat surface), and this increase in solubility can in turn affect the thickness of the graphene layer.

[0207] Once the powdered covetic material 2710 has been collected in the collection container, it can be further processed using conventional techniques (such as injection molding or other techniques using powdered metals). [, Use powder , ] [, covetic , ] [, Materials manufacturing technology , ] [, , ]

[0208] Figure 28 illustrates a method for manufacturing components from powdered covetic materials using injection molding technology. As shown, the method begins after a set of properties is collected for the component to be used in a specific application and / or environment (operation 2810), and then a specific powdered covetic material is selected based on at least one of the properties for that application or environment (operation 2820). This selection may be based on the desired mechanical properties of the component, and / or on the desired corrosion resistance of the component in the environment corresponding to its intended use, and / or other desired properties. The selection may be based on multiple desired properties, and in some cases, the selection tool addresses an optimization problem based on a set of properties and an objective function.

[0209] Once the covetic material is selected (operation 2820), the selected powdered covetic material (operation 2825) is melted (operation 2830) and introduced into the mold (operation 2840). The mold is maintained at a specified temperature and pressure for a specified duration (operation 2850), after which the temperature and pressure within the mold reach approximately 30°C and approximately atmospheric pressure (operation 2860). The component is then released from the mold (operation 2870) and deployed in the intended application (operation 2880).

[0210] As mentioned earlier, the selection of a specific covetic material can be based on a variety of desired properties, some of which can be used as variables in the objective function. In some cases, the selection of a specific covetic material can be based on specific principal properties (such as mechanical strength, weight, corrosion resistance, etc.). In other cases, the property of interest is the ratio of other properties, such as strength:weight, specific heat:weight, etc. In still other cases, the principal property will be maximized (or minimized) under one or more constraints on other properties.

[0211] Thus, powdered covetic materials can be deployed in a wide range of applications. In many cases, components made from powdered covetic materials are superior to those made from other materials. Some illustrative applications related to certain key properties are shown and discussed in Figure 29 below.

[0212] Figure 29 is Table 2900, which describes various properties of covetic materials. The properties shown include mechanical properties, thermal conductivity, oxidation resistance, durability, high-temperature softening resistance, fatigue resistance, and electrical conductivity. Individual parameters and / or combinations of these parameters become dominant in selecting a specific covetic material for a particular application.

[0213] As an example, when selecting a covetic material for manufacturing a corrosion-resistant valve, oxidation resistance can be a primary parameter. As another example, when selecting a specific covetic material for manufacturing turbine blades for an aircraft engine, mechanical properties such as the strength-to-weight ratio, which are subject to minimum strength constraints, can be primary mechanical properties. The blade may also need to exhibit very high fatigue resistance.

[0214] Typically, covetic materials not only exhibit the aforementioned properties but also have a lower density than the metals or alloys used in the manufacture of covetic powders. This lower density often corresponds to a lower weight of the resulting component compared to the same component made from a metal or alloy in the absence of carbon loading. Thus, truck components (such as the cab components shown), automobile components (such as door fenders, roof panels, etc.), motorcycle components, bicycle components, and various components of air vehicles (such as structural members) and / or water vehicles and / or airborne vehicles or platforms can utilize covetic materials with a lower weight-to-strength ratio compared to the base metals or alloys used in their manufacture.

[0215] As another example, covetic materials often exhibit excellent thermal conductivity, making structural components formed from covetic materials suitable for high-temperature applications (such as heat sinks for electronic devices, industrial heat exchangers, etc.).

[0216] As yet another example, covetic materials often exhibit exceptional corrosion resistance. More specifically, covetic laminates made using the aforementioned techniques demonstrate extremely high corrosion resistance, even at the top layers (such as the interface between the component and the environment). This property is particularly significant when components made from covetic materials are subjected to harsh environments.

[0217] As another example, covetic materials can be tuned for surface smoothness. More specifically, covetic laminates made using the aforementioned techniques exhibit extremely high surface smoothness. This surface smoothness property is particularly meaningful when covetic materials are used as thermal shielding components, such as in applications where friction at the surface (e.g., friction generated when fluid flows over a surface at high speed) may generate harmful heat. By using the techniques disclosed herein, specific compositions of covetic materials and / or specific techniques disclosed herein for depositing covetic materials can produce hydrosmolyzed surfaces, which can then be used in air vehicles and / or space-based vehicles.

[0218] In some implementations, a set of properties can dominate other properties. For example, the surface of a space-based vehicle (such as a satellite) may need to be substantially non-reflective of a certain range of electromagnetic radiation (e.g., substantially non-reflective of visible light), while at the same time, the surface of a space-based vehicle may need to be thermally insulated (e.g., non-conductive). The tuning techniques described above are applicable to such cases, where specific desired properties (such as non-reflectivity) dominate the tuning of the conductive paste spraying torch in order to produce a substantially non-reflective surface, even at the expense of other properties.

[0219] The properties shown and described in Figure 29 are merely examples. Additional properties and / or combinations of properties may be necessary or desired in various applications, and such additional properties are exhibited in the resulting material based on input tuning and control of the plasma spraying torch. As examples of the aforementioned additional properties only, such properties and / or combinations of properties may include or be related to the following: strength-weight metric, and / or specific density, and / or mechanical toughness, and / or shear strength, and / or flexural strength, etc.

[0220] For some applications (e.g., for high-stress / high-temperature operation, or operation in harsh chemical environments), there are specific specifications for the corrosion resistance, and / or strength, and / or hardness, and / or other properties of the final material or component. In some cases, these specific specifications can be met by using an alloy, which is then used to form components corresponding to the specific application. VIM furnaces are commonly used to form alloys. Sometimes, carbonaceous materials in powder form are added to the alloy mixture to reduce weight while maintaining the alloy's strength and / or other properties.

[0221] Unfortunately, the VIM furnace generates a strong magnetic field. This strong magnetic field typically has a stronger effect on the composition of the powder than gravity. Therefore, this magnetic field has a detrimental effect, causing powder to be ejected from the VIM furnace, even before the powder has a chance to enter the crucible of the VIM furnace, melt, and subsequently disperse in the molten mixture. One technique to address this detrimental ejection of powder from the VIM furnace is to granulate the powder into a dense form, so that when introduced into the VIM furnace, it is not ejected due to the furnace's magnetic force. Instead, the granular form enters the crucible of the VIM furnace, allowing it to melt inside the furnace and preventing it from mixing into the molten mixture.

[0222] Therefore, a carbon-containing alloy is formed, preferably a carbon-containing alloy having at least some (more preferably all) of the physical properties described above regarding covetic materials. Such physical properties should be understood to include, but are not limited to, high carbon loading (e.g., according to various embodiments, greater than 1.5%, greater than 5%, greater than 15%, greater than 40%, greater than 60%, and up to 90% carbon in the material); carbon substantially uniformly dispersed in the surface layer and / or bulk of the material; carbon present at interstitial sites in the lattice of metals alloyed with carbon; and a lack of carbon aggregates and / or agglomerates at the grain boundaries of the material.

[0223] Figures 30A1 and 30A2 depict the problems and solutions associated with molten powdered metallic decorative carbon compared to molten pellet form. These figures are presented side by side to specifically illustrate the problems (30A100) and solutions (30A200) associated with the use of powder in VIM processors.

[0224] As is known in the art, vacuum induction melting relies on a high-power current generating source 3006 to melt metal within a vacuum environment 3002. The induction heating process generates eddy currents within the conductor (e.g., metal). These eddy currents then generate heat. A magnetic field generated by the heated coil produces an upward force. Each individual particle of powder 3004 is not heavy enough to overcome the upward force generated by the electromagnetic field, resulting in harmful ejection 3003 of the metal decorative carbon powder. Figure 30A2 depicts the solution disclosed herein to this harmful ejection, namely, by compressing many individual particles of powder into pellets 3008. Thus, gravity acting on the pellets overcomes the force of the magnetic field on the powder components. This solves the aforementioned problem that the magnetic field of the VIM processor acts on the powder more strongly than gravity. Therefore, the pellets enter the crucible and are heated together with the components of the mixture.

[0225] Once the mixture reaches its melting point, the magnetic field begins to stir the metal alloy. The alloy melt—including the carbon-containing components dispersed in the molten alloy matrix—can now be poured into a component-specific mold for a given application.

[0226] Figure 31 illustrates a method for minimizing or eliminating material ejection during the introduction of pellets 3108 into the VIM processor 3110. This figure is presented to illustrate an exemplary material handling process for granulating powdered material 3004 prior to its use in the VIM processor. In alternative methods, the VIM processor 3110 may be used in place of or in combination with vacuum arc melt processing equipment, electron beam furnaces, ion plating furnaces, plasma flame sources, smelting furnaces, conventional metal-to-metal melting furnaces, or any equivalents and / or components thereof that will be understood by one generally skilled in the art upon reading this disclosure.

[0227] To obtain a powdered material, a supply gas (e.g., a hydrocarbon, such as methane) is fed into a plasma reactor to produce a plasma containing dissociated carbon and hydrogen atoms. At a specific location in the plasma plume, such as where the hydrogen and carbon atoms are completely dissociated, a molten metal (e.g., molten nickel) is injected into the plasma. The injected molten metal combines with the dissociated carbon atoms to form metallic decorative carbon molecules, some of which merge with other metallic decorative carbon molecules. When cooled to a temperature below the melting point of the injected metal, the precipitate exits the plasma reactor as a powdered material 3104.

[0228] After collecting the metallic decorative carbon powder from the plasma reactor (step 3114), the metallic decorative carbon molecules may be separated from dissociated hydrogen molecules (e.g., H2) in a gas-solid separator or other collection container located at the outlet of the plasma reactor. For example, and as shown, as those skilled in the art will understand after reading this disclosure, the gas-solid separator container 3102 can be implemented using equipment such as gravity separators, cyclone separators, scrubbers, electrostatic separators, filters, etc.

[0229] In the example shown, metallic decorative carbon (solid) and hydrogen molecules (gas) can be placed in a cyclone gas-solid separator container 3102. This particular configuration uses the concept of inertia to separate the solid (e.g., metallic decorative carbon) from the gas (e.g., hydrogen). Due to the molecular weight difference between the metallic decorative carbon and hydrogen, the lighter material (hydrogen in this case) will be more affected by the vortices generated within the cyclone gas-solid separator container. Therefore, the hydrogen will be forced (by cyclone action) upwards, thus separating the gas from the heavier powdery material 3104 (e.g., metallic decorative carbon molecules). The shape of the gas-solid separator container facilitates the downward flow of the metallic decorative carbon particles towards the bottom of the container. This downward flow is opposite to the upward flow of the hydrogen. Therefore, the metallic decorative carbon particles can be collected for further processing.

[0230] Once the metallic decorative carbon powder has been isolated from and trapped by hydrogen, the metallic decorative carbon is compressed to form rigid bulk pellets 3108 (step 3116). This granulation can be accomplished, for example, by using a granulator 3106, such as a 12-ton press that is automatically actuated or manually operated. Although this example illustrates the use of a 12-ton press as granulator 3106, any granulation techniques and / or equipment suitable for producing pellets with sufficient mass to avoid ejection from the VIM processor can be used without departing from the scope of the invention.

[0231] The granulation of metallic decorative carbon utilizes the mechanics of how the granulated metallic carbon and the magnetic flux of VIM interact under gravity. More specifically, gravity has a stronger effect on the pellets than magnetic flux. Therefore, when pellets (rather than powder) are introduced into the VIM processor 3110, the aforementioned problem of material ejection due to magnetic force is eliminated.

[0232] Once the pellets are introduced into the crucible of the VIM processor, they begin to melt and mix with the other contents of the crucible (step 3118). During this step, as the pellets melt, they are uniformly dispersed within the metal mixture. To promote uniform dispersion, the VIM crucible may be individually loaded with the pellets, wherein, according to various embodiments, the pellets are placed on top of the metal powder, or the metal powder is placed both below and above the pellets.

[0233] The resulting melt 3112 can then be poured into a mold (step 3120) and / or used in conjunction with injection molding equipment to form components (e.g., turbine blades, automotive components, medical devices, etc.). In some cases, the output of the VIM processor (e.g., melt 3112) is cooled and subsequently powdered using any suitable equipment for use with other mechanical part forming methods (e.g., 3D printing) and subsequently in any application (step 3122).

[0234] Figure 32 depicts melt 3112 placed in mold 3202. Melt 3112 can be placed in mold 3202 of any shape or form. Once the melt has cooled, the component can be removed from the mold and used in its intended application.

[0235] As an example, a mold for turbine blades can be used. A melt consisting of a metal mixture and carbonaceous components can then be placed into the turbine blade mold and cooled. Once cooled and removed from the mold, the turbine blade is ready for use in its intended application. As another example, the melt can be cooled, then powdered, and then packaged for use in 3D printers or other additive manufacturing technologies / equipment.

[0236] Figure 33 illustrates a simplified schematic diagram of pellet processing according to various methods. As described in detail above with reference to Figure 31, a powdered material 3104 is obtained, for example, as an output from a microwave plasma reactor, separated from unwanted gases, and pressed into pellets using a pelletizer 3106. Preferably, the pelletizer 3106 includes a die whose physical configuration / arrangement is suitable for producing pellets with the desired geometry. As shown in Figure 33, the die 3106a is configured to produce generally cylindrical pellets (or "bulbs") with a diameter of about 1 cm. Of course, those skilled in the art will understand that the geometric characteristics of the pellets can be selected and / or adjusted based on the properties (e.g., magnetic field strength, volume, etc.) of the VIM processor (or equivalent device) to be used to produce the desired material. It is noteworthy that the pellets produced according to the experiment presented in Figure 33 can be produced without chemical binders.

[0237] As shown in Figure 33, and experimentally demonstrated, the present invention successfully produces pellets composed essentially only of natural graphene (3108a) and pellets formed of metallic decorative carbon (e.g., decorative graphene) (3108b). Both types of pellets can be produced using substantially the same technique, the only difference being the composition of the powder used to produce the pellets.

[0238] In another experiment, schematically illustrated in Figure 34, pellets (such as pellet 3108) were dispersed in an isopropanol solution by manual stirring. After stirring, which can be performed manually or using an ultrasonic rod (or other mechanism for ultrasonic stirring), the resulting suspension exhibited permeability, as will be understood by one skilled in the art upon reading this disclosure. Magnetic test 2 verified the dispersion of nickel-decorated carbon. Inventive concept

[0239] Various embodiments, styles, features, advantages, implementation methods, configurations, and arrangements of the inventive concept have been described above with reference to the figures. It should be understood that, unless otherwise expressly stated herein, such embodiments, styles, features, etc., can be combined or modified in any suitable manner that a person generally skilled in the art would understand after reading this disclosure, without departing from the scope of this disclosure. It is quite clear that the following inventive concepts exist in the preferred features, configurations, etc., of the inventive concepts presented herein, and can be used in any suitable manner, combination, or arrangement, while still remaining within the scope of this invention.

[0240] According to one embodiment, a material composition comprises one or more particles, and at least some of these particles independently comprise a metal lattice having one or more coherent planar graphene layers disposed therein. At least some carbon atoms of the one or more coherent planar graphene layers may be disposed in interstitial sites of the metal lattice. For example, the one or more coherent planar graphene layers may be partially or completely interstitially interspersed between the basal planes of the metal lattice. Preferably, the metal lattice comprises about 15 wt% to about 90 wt% carbon, and about 15% to about 60 wt% of carbon in the particles are present at their interstitial sites. Furthermore, in some methods, the metal lattice is characterized by a crystal structure selected from face-centered cubic (FCC), body-centered cubic (BCC), and hexagonal close-packed (HCC). In some methods, the one or more coherent planar graphene layers consist of a single layer of graphene. Alternatively, the one or more coherent planar graphene layers comprise at least five graphene layers and no more than fifteen graphene layers. According to the selected embodiment, each of the one or more coherent planar graphene layers is independently and substantially defect-free. The metal lattice may comprise one or more metals selected from the group consisting of: aluminum, copper, iron, nickel, titanium, tantalum, tungsten, chromium, molybdenum, cobalt, manganese, niobium, and combinations thereof. For example, the metal lattice may be an inconel alloy or include inconel alloys, and the inconel alloy may be a superalloy formed from one or more metals selected from the group consisting of: nickel, chromium, aluminum, copper, iron, titanium, tantalum, molybdenum, cobalt, manganese, and niobium. Furthermore, the inconel alloy may be selected from the group consisting of: Inconel 600, Inconel 617, Inconel 625, Inconel 690, Inconel 718, and Inconel X-750. At least some carbon atoms in the one or more graphene layers are preferably covalently bonded to metal atoms in the metal lattice. More preferably, the covalent bonds between the carbon atoms of the graphene and the metal atoms include nonpolar covalent bonds. Similarly, at least some carbon atoms in the one or more graphene layers may be covalently bonded to other carbon atoms in the one or more graphene layers, and some or all of the covalent bonds between the carbon atoms of the graphene may include nonpolar covalent bonds. Continuing with reference to the bonding within the material composition, the one or more particles may completely or substantially exclude polar covalent bonds. Furthermore, the metal lattice of each of the one or more particles substantially or completely excludes ionic bonds. "Substantially" should be understood to mean a composition in which any polar bonds, ionic bonds, or other bonds of the aforementioned types present in the composition have no effect or a negligible effect on the structural, physical, and functional properties of the material composition. The particles may be characterized by the absence of carbon aggregates and / or agglomerates at their grain boundaries, a diameter in the range of about 20 nm to about 3.5 μm, being compressed into pellets, or any combination of these characteristics.Depending on certain morphologies, the maximum identifiable feature size of this material composition is in the range of about 0.1 nm to about 1 µm. These particles can be compressed into pellets.

[0241] In the foregoing specification, this disclosure has been described with reference to specific embodiments thereof. However, it is apparent that various modifications and changes can be made to it without departing from the broader spirit and scope of this disclosure. For example, the process flow described above is based on a specific sequence of process actions. However, the sequence of many process actions described may be changed without affecting the scope or operation of this disclosure. This specification and accompanying drawings are intended to be illustrative and not restrictive.

[0242] 105: Images 106: Homogeneous image 114: High-resolution transmission electron microscopy images 116: High-resolution energy-dispersive X-ray image 500: Dual Plasma Torch Equipment 600: Pulse Microwave Plasma Spraying Torch Equipment 604: Additional Port 605: Hydrocarbon Process Gases 900: Scanning electron microscope image 1100: Plasma Flame Equipment 1202: Process Gas Port 12031: Additional Port 12032: Additional port 1204: Entrance 1300: Pulse Microwave Plasma Spraying Waveguide Equipment 1600: Plasma spraying equipment 1700: Surface Wave Plasma System 1803: Growth plate 1810: Axial Field Configuration 1812: Input gas 1814: Plasma Flame 1816:Substrate 1818: Metallic and / or carbon particles 1820: Radial Field Configuration 1821: Acceleration Zone 1822: Microwave Energy 1823: Collision Zone 1824: Quenched layer 1862: Input Port 2052: Carbon 2054: Copper 2062: Top surface region 2064: Covetic material region 2066: Body Metal Region 2072: Regions with higher carbon content 2074: Region with higher metal content 2104: First Region 2106: Second Region 2108: Molten Metal 2110: Outlet of microwave reactor 2112: Spray coating materials 2114: The obtained sedimentary material 2116: Target substrate 2209: Melting equipment 2310:Flexible substrate 26E00: Covetic material 27A00: Exemplary apparatus for producing powdered covetic materials 27B00: Fluidized bed equipment 2702: Cooling Area 2704: Collection Container 2710: Powdered covetic material 2750: Fluidized Bed 2752: Power Supply 27561: First powder 27562: Second powder 2760: Heat source 2762: Conical Body 3002: Vacuum environment 3004: Powdered material 3006: High-power current generator 3008: Pellet 3102: Gas-solid separator container 3104: Powdered material 3106: Granulator 3106a: Mold 3108: Granules 3108a: Natural graphene 3108b: Metallic Decorative Carbon 3110: VIM Processor 3112: The obtained melt 3202: Mold

Claims

1. A material composition comprising one or more particles, wherein the one or more particles independently comprise a metal lattice in which graphene is disposed at interstitial positions.

2. The material composition of claim 1, wherein at least some of the graphene is characterized as having a structure having one or more coherent planar layers.

3. The material composition of claim 1, wherein at least some of the graphene is interspersed between the basal planes of the metal lattice.

4. The material composition of claim 1, wherein the graphene is substantially free of crystal defects.

5. The material composition of claim 1, wherein the one or more particles are characterized by the absence of carbon aggregates and / or carbon agglomerates at their grain edges.

6. The material composition of claim 1, wherein the one or more particles independently comprise about 15 wt% to about 90 wt% carbon; and wherein the metal lattice comprises about 15 wt% to about 60 wt% carbon at its interstitial sites.

7. The material composition of claim 1, wherein at least some of the graphene is original.

8. A material composition comprising one or more particles, wherein the one or more particles independently comprise a metal lattice in which graphene is disposed; and wherein each particle is characterized by the absence of carbon aggregates and / or carbon agglomerates at its grain edges.

9. The material composition of claim 8, wherein at least some of the graphene is characterized as having a structure having one or more coherent planar layers.

10. The material composition of claim 8, wherein at least some of the graphene is disposed in interstitial positions in the metal lattice.

11. The material composition of claim 8, wherein at least some of the graphene is interspersed between the basal planes of the metal lattice.

12. The material composition of claim 8, wherein the graphene is substantially free of crystal defects.

13. The material composition of claim 8, wherein the one or more particles independently comprise about 15 wt% to about 90 wt% carbon; and wherein the metal lattice comprises about 15 wt% to about 60 wt% carbon at its interstitial sites.

14. The material composition of claim 8, wherein at least some of the graphene is primitive.

15. A material composition comprising one or more particles, wherein the one or more particles independently comprise a metal lattice in which graphene is disposed; and wherein the graphene is substantially free of crystal defects.

16. The material composition of claim 15, wherein at least some of the graphene is characterized as having a structure having one or more coherent planar layers.

17. The material composition of claim 15, wherein at least some of the graphene is disposed in interstitial positions in the metal lattice.

18. The material composition of claim 15, wherein at least some of the graphene is interspersed between the basal planes of the metal lattice.

19. The material composition of claim 15, wherein the one or more particles are characterized by the absence of carbon aggregates and / or carbon agglomerates at their grain edges.

20. The material composition of claim 15, wherein the one or more particles independently comprise about 15 wt% to about 90 wt% carbon; and wherein the metal lattice comprises about 15 wt% to about 60 wt% carbon at its interstitial sites.

21. The material composition of claim 15, wherein at least some of the graphene is original.

Images