Methods for producing graphene, other carbon allotropes and carbon materials

Abstract

Methods and systems for the synthesis of graphene, synthetic graphite, and other carbon allotropes are described. Accordingly, the present methods describe a method for synthesizing carbon nanostructures and synthetic graphite by using non-recyclable materials (non-recyclable carbon), such as waste plastics (i.e., polypropylene, styrene, polyethylene, polyvinyl chloride, PVDF, tires, etc.), liquid waste (i.e., distillation residues, PVDF liquid foam, contaminated oil, etc.), regardless of their condition, cleanliness, or whether they are contaminated with other by-products.

Description

[Technical Field]

[0001] Cross-references to related information This application claims the benefit of U.S. Patent Application No. 63 / 439,463, filed January 17, 2023, and entitled "Process for Producing Graphene, Other Carbon Allotropes and Materials," the contents of which are incorporated herein by reference in their entirety. This application is a continuation-in-part of U.S. Patent Application Serial No. 17 / 750,613, filed May 23, 2022, and entitled "Gasification or Liquefaction of Coal Using a Metal Reactant Alloy Composition," which is a continuation-in-part of U.S. Patent Application Serial No. 16 / 434,771, now U.S. Patent No. 11,359,253, filed June 7, 2019, and entitled "Gasification or Liquefaction of Coal Using a Metal Reactant Alloy Composition," which is a continuation-in-part of U.S. Patent Application Serial No. 16 / 434,771, now U.S. Patent No. 11,359,253, filed December 17, 2015, and entitled "Gasification or Liquefaction of Coal Using a Metal Reactant Alloy Composition." No. 14 / 973,243, now U.S. Pat. No. 10,316,375, filed Jun. 4, 2012, entitled "Gasification or Liquefaction of Coal Using a Metal Reactant Alloy Composition," which is a continuation of U.S. Pat. Appl. No. 13 / 487,430, now U.S. Pat. No. 9,216,905, filed Jun. 4, 2012, entitled "Gasification or Liquefaction of Coal Using a Metal Reactant Alloy Composition," which claims the benefit of U.S. Provisional Patent Application No. 61 / 493,247, filed Jun. 3, 2011, entitled "Gasification or Liquefaction of Coal Using a Metal Reactant Alloy Composition," the contents of which are incorporated herein by reference in their entirety.

[0002] The present disclosure relates generally to the technical field of synthesis of graphene, synthetic graphite, and other carbon allotropes. [Background technology]

[0003] The synthesis of carbon allotropes, including graphene, is highly dependent on carbon sources such as high-purity gases, graphite, and other organic carbon sources. Similarly, the purity of the metal or metal mixture involved in the synthesis of carbon nanomaterials plays an important role in the reaction yield and crystallinity of the nanomaterials. Graphene was originally isolated as a monolayer of graphite and obtained by mechanical exfoliation. Graphene oxide (GO) was further isolated as the oxidation product of graphite, while reduced graphene oxide (RGO) was obtained by the reaction of GO with a reducing agent. Graphene now more precisely refers to a class of nanomaterials, including: nanoplatelets (GNPs), few-layer graphene (FLG), single-layer graphene (SLG), multilayer graphene (MLG), graphene oxide (GO), and reduced graphene oxide (RGO). Many techniques have been developed for the synthesis of graphene, including chemical exfoliation, chemical vapor deposition (CVD), thermal plasma, flash growth, electrochemical exfoliation, micromechanical exfoliation, laser ablation, ignition chamber, and pyrolysis. These techniques are compatible with different carbon sources and may or may not require metals as catalysts. Techniques such as CVD, thermal plasma, laser ablation, ignition chamber, and flash growth can produce highly crystalline graphene of single or few layers. Nevertheless, each of these techniques requires a high-voltage discharge, which requires highly controlled conditions, in addition to controlled atmospheres and high-purity gases containing hydrogen and / or oxygen. Similarly, synthetic graphite is primarily obtained by the Hazor process, which is the chemical decomposition of methane catalyzed by iron ore. Additionally, other petroleum derivatives are used to produce synthetic graphite. Current methods for synthesizing carbon nanostructures or synthetic graphite all rely on traditional carbon and catalyst sources, but still require non-recyclable carbon precursor materials and metals. Summary of the Invention

[0004] One embodiment of the present disclosure includes a method for producing a carbon material, the method comprising combining a carbon precursor and a catalyst in a controlled, oxygen-free environment, and carrying out the reaction at a temperature ranging from about 600°C to 1400°C. Another embodiment of the present disclosure contemplates a method for synthesizing carbon, the method including the steps of: combining a feedstock with molten aluminum; injecting the mixture of molten aluminum and feedstock into a reaction vessel containing additional molten aluminum, where the injection occurs below the surface of the molten aluminum in the reaction vessel; and reacting the feedstock with the molten aluminum to form one or more carbon-containing products. Another embodiment of the present disclosure is a reactor vessel for reacting a carbon precursor with molten metal. The reactor vessel comprises a reactor wall, a refractory material lining the inside of the reactor wall, and a cooling plate attached to the outside of the reactor wall, the cooling plate forming a cooling fluid flow path between the cooling plate and the reactor wall. The reactor vessel further comprises an aluminum supply line passing to the reactor wall; an inlet line passing through the reactor wall and having an outlet within the reactor vessel, the inlet line configured to deliver the carbon precursor to the reactor vessel; and one or more withdrawal lines passing through the reactor wall and configured to withdraw one or more output products. This Summary is provided to introduce some concepts in a simplified form that are further described below in the Detailed Description. This Summary is not intended to identify key features or essential features of the claimed subject matter, nor is it intended to be used as an indicator of the scope of the claimed subject matter.

[0005] For a more complete understanding of the present disclosure, reference is now made to the following descriptions taken in conjunction with the accompanying drawings, in which: [Brief explanation of the drawings]

[0006] [Figure 1] 1 illustrates a basic process flow and system embodiment. [Figure 2] 1 illustrates an embodiment of a reaction vessel of the present disclosure. [Figure 3] 1 shows a detailed cross section of the reactor vessel wall. [Figure 4] 1 shows an embodiment of an improved reaction vessel incorporating a vortex. [Figures 5A-5N] This shows an SEM image of a sample (ER-01) treated at 900-950°C using non-recyclable plastics (HDPE, PET, PP, styrene, PVC) and tires (waste plastics) as carbon precursors and aluminum alloy as a catalyst. [Figures 6A-6N] TEM images of a sample (ER-01) treated at 900-950 °C using non-recyclable plastic as a carbon precursor and aluminum alloy as a catalyst. Images (j) and (n) show the diffraction results (SAED) of graphene sheets. [Figure 7] This shows the Raman spectrum of sample ER-01, which was treated at 900-950°C using waste plastic as a carbon precursor and aluminum alloy as a catalyst. [Figure 8] 1 shows the thermogravimetric analysis (TGA) results of sample ER-01 in synthetic air. [Figure 9] 1 shows the TGA results of sample ER-01 in argon. [Figure 10] 1 shows the XPS spectrum of carbon of sample ER-01. [Figures 11A-11H] Shown is an SEM image of sample ER-02, which was processed at approximately 900-1100 °C using natural gas as the carbon precursor and aluminum alloy as the catalyst. [Figure 12] This shows an SEM mapping image of sample ER-02, which was processed at approximately 900-1100 °C using natural gas as the carbon precursor and aluminum alloy as the catalyst. [Figures 13A-13F]TEM image of sample ER-02, which was treated at 900-1100 °C using natural gas as the carbon precursor and aluminum alloy as the catalyst. [Figure 14] The Raman spectra of samples treated at approximately 900-1100 °C using natural gas as the carbon precursor and aluminum alloy as the catalyst are shown. [Figures 15A-15I] This shows an SEM image of sample ER-03, which was treated at approximately 900-950 °C using HDPE as the carbon precursor and an aluminum alloy as the catalyst. [Figure 16] SEM mapping of sample ER-03, which was treated at approximately 900-950 °C using HDPE as the carbon precursor and aluminum alloy as the catalyst, is shown. [Figure 17] The EDS spectrum of the analyzed area is shown. [Figures 18A-18C] EDS mapping of carbon, oxygen, and sulfur is shown. [Figure 19] This shows the Raman spectrum of a sample treated at approximately 900-950°C using HDPE as the carbon precursor and an aluminum alloy as the catalyst. [Figure 20] The TGA results for sample ER-03 are shown. [Figure 21] 1 illustrates one embodiment of the method of the present disclosure. [Figure 22] 1 illustrates one embodiment of the method of the present disclosure. DETAILED DESCRIPTION OF THE INVENTION

[0007] Before describing various embodiments of the present disclosure in detail, it should be understood that the present disclosure is not limited to the parameters of the particularly exemplified systems, methods, apparatus, products, processes, and / or kits, which may, of course, vary. Accordingly, while particular embodiments of the present disclosure will be described in detail with reference to particular configurations, parameters, components, elements, etc., the description is illustrative and should not be construed as limiting the scope of the claimed embodiments. Moreover, the terminology used herein is for the purpose of describing the embodiments and is not necessarily intended to limit the scope of the claimed embodiments. As described above, several challenges currently exist in the field of graphene, graphite, and carbon allotrope synthesis. There is a continuing need to develop alternative methods for producing carbon nanostructures (e.g., graphene, carbon nanotubes, etc.) and synthetic graphene using non-recyclable carbon and metals under conditions that are applicable to industrial scale. Certain aspects of the present disclosure and its embodiments may provide solutions to these and other problems. The present disclosure provides various processes and systems for recycling plastics, electronics, munitions, coal, coke, or propellants, and / or for producing graphene, graphite, and other carbon allotropes. Various embodiments may utilize a molten aluminum or aluminum alloy bath. Certain embodiments utilize a molten aluminum bath as a reactant. The pulverized feedstock is introduced below the surface of the molten aluminum bath and reacts with the aluminum to decompose the feedstock. In this process, elemental carbon, sulfur, copper, iron, and rare earth and heavy metals, as well as molecular hydrogen, nitrogen, methane, and other hydrocarbons, can be removed from the molten bath. The product can be sold, and the nitrogen can be released to the environment or captured. Certain embodiments may provide one or more of the following technical advantages: Advantages include (re)capture of various materials, all of which can be reused and / or sold, potentially making the described embodiments a truly "green" zero-waste solution.

[0008] Some of the embodiments contemplated herein will now be described more fully with reference to the accompanying drawings, in which: The embodiments are provided for purposes of illustration, to convey the scope of the subject matter to those skilled in the art. Certain embodiments utilize a molten metal, such as an aluminum or aluminum alloy bath, as the primary reactant. The aluminum may also be alloyed with other elements, including, but not limited to, zinc, iron, copper, silicon, and calcium. Other metals and metal alloys, such as calcium and silicon, are also contemplated. The flue gas stream contains oxygen containing greenhouse gases generated by the combustion process, and the oxygen-containing gases are removed from the flue gas stream by passing it through an aluminum alloy bath. The process can generate excess heat that can be used to facilitate other processes, such as the cogeneration of electricity. The amount of excess heat generated in the process varies depending on the carbon precursor feedstock or the composition of the gases in the feedstock. If the feedstock contains other compounds, these compounds may also be decomposed or captured. For example, if the feedstock contains inorganic compounds such as chlorine, the process will produce aluminum salts (in this case, aluminum chloride). The present disclosure also provides methods and systems for capturing heavy metals (such as, but not limited to, mercury) or rare earth metals. These heavy metals are often found in consumer electronics or munitions. In this process, a molten metal bath decomposes metal compounds introduced into the molten metal bath. As additional aluminum is added to the bath, the heavy metals settle to the bottom of the reaction vessel and are removed from the reaction vessel. The heavy metals removed from the bottom of the reaction vessel may have some entrained aluminum, which can be removed and purified, allowing the heavy metals to be captured.

[0009] 1 shows one embodiment 100 contemplated by this disclosure. In the basic process, pulverized material is introduced below the surface of a molten metal bath 103 through a feed line 102 using an injection feed system 101. Elemental species such as carbon, sulfur, etc. are captured 104, less dense secondary compounds are removed from the bath surface 105, and more dense secondary compounds are removed from the bath bottom 106. While this is described as a method for recycling plastics, electronics, munitions, or propellants, it is also contemplated to use this method to recycle other organic compounds, such as, but not limited to, rubber, coal, coke, oil, tar, etc.

[0010] FIG. 2 illustrates another contemplated process flow embodiment 200. The process described addresses recycling plastics, electronics, munitions, propellants, and the like, but other materials can also be processed. Ground feedstock is introduced into the process through blower supply line 211. Blower 210, which can be another type of injection device, is used to inject the ground feedstock into reaction vessel 220 through injection line 212. Injection line 212 introduces the ground feedstock, entrained in an inert gas such as nitrogen or an active gas such as, but not limited to, hydrogen, propylene, or natural gas, below the surface of molten aluminum compound 226. Injection line 212 must be sufficiently below the surface of molten aluminum compound 226 to allow for adequate mixing. Heavy products of the reaction, typically the heavy metals listed above, settle within the reaction vessel. The reaction vessel typically has a sloping bottom, although other designs, such as a conical bottom, are also possible. Once the heavy products settle, they are recovered using an overhead recovery line, a pump, or recovery lines 223, 224, and 225. Recovery lines 223, 224, and 225 allow for removal of heavy metals of different densities. Depending on the size of the process, the heavy products can be removed continuously or a batch removal process can be used. Reaction vessel 220 also includes aluminum supply line 221. It is used to supply additional aluminum compounds to replenish those consumed in the reaction with the ground feedstock. Additional heat may be required, for example, during start-up. Heater 227 is provided for this purpose. Heater 227 can be any type of heater, such as radiant, inductive, or convective. For example, heater 227 can be a microwave heater or radio frequency heater tuned to the metal alloy being used.

[0011] Heat generated by the process is preferably removed. Cross-section A, detailed in Figure 3, illustrates one way heat can be removed from the process. Reaction vessel 220 is lined with refractory material 310, which protects vessel wall 320. A cooling plate 330 is attached to vessel wall 320, and a coolant (e.g., air, water, or other fluid) circulates through channels formed between cooling plate 330 and vessel wall 320. Insulation 340 surrounds the cooling plate for safety purposes as well as to maximize heat recovery. After cooling water captures the heat generated from the process, it can be sent to a cooling tower or the heat can be recovered and used for other purposes. If this process is used in a facility that requires a hot water source, a heat recovery system can be designed for that purpose. However, the heat can also be used to generate electricity.

[0012] Returning to FIG. 2, a steam turbine power generation process is shown. In this case, cooling water is introduced through cooling feed 228. As the cooling water moves around the reactor vessel 220, it picks up heat and generates steam. The generated steam is then sent to steam turbine 232 via steam line 229. The steam passes through the turbine and, as it condenses, rotates the turbine blades of turbine 232. Turbine 232 is coupled to generator 231. The turbine rotates the rotor of generator 231 via a stator, generating electricity. While this process will only be briefly described, this steam turbine power generation process is well known in the art, and any steam turbine power generation process may be utilized. As noted above, the reaction may also produce materials such as elemental carbon, elemental sulfur, molecular nitrogen, and molecular hydrogen. These materials can be removed from the reaction vessel using blower 250. Blower 250 can, for example, draw hot elemental carbon, elemental sulfur, molecular nitrogen, and molecular hydrogen from reaction vessel 220 through heat exchanger feed line 241 and into heat exchanger 240. Heat exchanger 240 then cools the materials, allowing for further processing. The hydrocarbons produced can also be condensed in heat exchanger 240. These liquid hydrocarbons can be recovered for further use or sale. While heat exchanger 240 can be any heat exchanger, in a preferred embodiment, heat exchanger 240 is a forced air heat exchanger. However, other heat exchangers are also contemplated. The process stream then exits the heat exchanger through line 242 and enters two cyclone separators through blower 250 and blower discharge line 252. The first separator 260 separates the carbon from the process stream. The carbon is recovered through separation line 263. The remaining process stream proceeds to a second separator 270, which separates the sulfur from the process stream. Once the process stream has cooled to below 444°C, a cold finger can be used to remove the sulfur. The sulfur is recovered through separation line 273. The remaining process stream (which may include gaseous nitrogen and hydrogen) is then separated in a cryo-unit 280, where the gas stream is further cooled to allow for separation of the components.

[0013] Below is a non-exhaustive list of potentially recycled ground feedstocks and the elemental products produced by reaction in the molten metal bath: Polyvinyl chloride: 2(C2H3Cl)n → 4C + 3H2 + 2Cl Polypropylene: (C3H6)n → 3C + 3H2 PET: (C10H8O4)n → 10C + 4H2 + 2O2 Polycarbonate: (C16H14O3)n → 16C + 7H2 + 30O2 ABS:(C8H8・C4H6・C3H3N)n→15C+17 / 2H2+1N 4-(tert-butyl)styrene (butylstyrene): (CH3)3C6H4CH=CH2 → 12C + 8H2 Nylon 66: (C12H22N2O2)n → 12C + 11H2 + 2N + 2O2 Dibutyl phthalate: 3C16H22O4 + 8Al = 48C + 33H2 + 4Al2O3 Diphenylamine: 2C12H11N+0Al = 24C+22H2+N2 Nitrocellulose: 6C6H9(NO2)O5+12Al=36C+27H2+3N2+6Al2O3 2C6H9(NO2)2O5+12Al=12C+9H2+N2+6Al2O3 6C6H9(NO2)3O544Al=36C+27H2+9N2+22Al2O3 Dinitrotoluene: 3C7H6N2O4 + 8Al = 21C + 9H2 + 3N2 + 4Al2O3

[0014] FIG. 4 illustrates another contemplated embodiment. It shows an improved process flow 400 using a vortex entry. Similar to the process described in FIG. 2, the improved process allows for the recycling of, for example, plastics, electronics, coal, coke, munitions, or propellants. Instead of being injected directly into the aluminum bath, the ground feedstock is introduced to the process through a line fed by a vortex 402. The vortex 402 is formed in a ceramic bowl 415 by pumping in molten aluminum or aluminum alloy. The molten aluminum or aluminum alloy can be added through a new aluminum input line 404 or recirculated from the aluminum bath using a pump 406. The ground feedstock (which may include any of the above materials requiring recycling) can then be introduced into the ceramic bowl 415 through a gravity feeder 405. The ground feedstock is mixed with the molten aluminum or aluminum alloy, and the mixture is drawn to the bottom of the bowl by the rotation of the vortex 402. The bottom of the ceramic bowl 415 may have a connection line 408 to an aluminum bath through which the mixture of ground feedstock and molten aluminum or aluminum alloy enters the aluminum bath. Another embodiment of the improved process flow 400 is similar to the flow shown in FIG. The vortex entry shown in FIG. 4 offers several advantages over other injection systems. The vortex improves mixing of the ground feedstock with the molten aluminum or aluminum alloy, resulting in a more efficient recycle reaction. Additionally, because the ground feedstock is already mixed with the molten aluminum in the ceramic bowl 415, the temperature of the mixture has had an opportunity to equalize, and its temperature can be relatively close to that of the molten aluminum in the bath. Therefore, using a vortex entry results in less localized cooling and a more consistent temperature gradient at the entry injection point. As described above, when the feedstock enters the aluminum bath or vortex, a reaction between the ground feedstock and the aluminum or aluminum alloy bath begins. The denser materials begin to settle, while the lighter materials rise. The lightest materials, such as gas, bubble to the surface where they are collected.

[0015] Other embodiments of the present disclosure may focus on the production of graphene, such as carbon nanostructures and synthetic graphite. One synthesis method for producing graphene may be defined by mixing a non-recyclable carbon precursor with a catalyst in a controlled, oxygen-free environment. The reaction is carried out at temperatures ranging from about 600°C to 1400°C. The apparatus or system used may be similar to those shown in Figures 1, 2, or 4. Such embodiments may be defined by the decomposition of a carbon precursor into carbon, hydrogen, and oxygen atoms, the latter if present in the precursor. Such a process may involve the epitaxial assembly of carbon atoms on the surface of liquid aluminum. The presence of oxygen during graphene synthesis may result in a doping process. To evaluate various approaches to graphene synthesis and to increase the graphitization level, several growth runs were performed, applying different reaction times and temperatures. Thus, the system may be designed to allow for the synthesis of various graphite or graphene structures by varying the residence time of the carbon precursor. Various different metal catalysts (e.g., Mg, Fe, Co) can be added to the catalyst to aid in the synthesis of different carbon isotopes. Reactor embodiments (e.g., the reactors in Figures 2 and 4) are currently designed to operate at relatively low pressures, approximately 3-5 psi gauge. It is envisioned that the reactor can be operated at higher pressures, up to several atmospheres. A carrier gas may or may not be used during the process. This carrier gas can be either a short-chain hydrocarbon, nitrogen, or hydrogen. An inert gas may or may not be used during the process. Currently, nitrogen is used as the inert gas in some exemplary embodiments, but argon or other inert gases can be used. Hydrogen may or may not be a by-product of the reaction. Further micronization, grinding, or jet milling can be used to reduce the size of any of the products and outputs of the process. Other methods may be used to functionalize the produced carbon. A combination of waste metals (e.g., Mg, Fe, Co, etc.) may be applied as a secondary catalyst in some embodiments. Synthesis of carbon nanostructures and synthetic graphite may occur while recycling other metals. In certain embodiments, synthesis of carbon nanostructures and synthetic graphite may occur in the presence of chalcogenides (e.g., oxygen, sulfur, selenium, tellurium).

[0016] Several experiments were performed to evaluate the graphene production capabilities of certain embodiments. Several samples were prepared according to Table 1 below. [Table 1]

[0017] Example 1 - Synthesis of graphene using waste plastic (Sample ER-01) In Example 1, non-recyclable crushed waste plastic was inserted into a reactor along with an aluminum alloy. An inert gas (e.g., nitrogen) was used as a carrier to transport graphene from the reaction chamber to a collection vessel. The temperature range of the reaction chamber was maintained between 600°C and 950°C. Sample ER-01 contained non-recyclable plastics (e.g., HDPE, PET, PP, styrene, PVC) and tires (waste plastics). These served as carbon precursors, and an aluminum alloy was used as a catalyst. Figures 5A-5N show scanning electron microscope (SEM) images of sample ER-01 after manual grinding. The sample was dispersed in methanol, sonicated in an ultrasonic bath for 5 minutes, and drop-cast onto a Si / SiO2 wafer. The images show agglomerations of particles larger than 5 μm, while high-resolution (×250,000) images reveal small flakes smaller than 100 nm. Figures 6A-6N show transmission electron microscopy (TEM) images of graphene sheets and ribbons (ER-01) after dispersion in methanol for 10 minutes using an ultrasonic bath. A droplet of the sample was deposited on a nickel TEM grid coated with lacey carbon. Figures 6A-6N show graphene flakes (images A-F) and sheets (images G-N). Selected-area electron diffraction (SAED) revealed that the graphene sheets possessed up to three turbostratic structures (images J and N). Figure 7 shows the Raman spectroscopy results for graphene (sample ER-01). The Raman spectrum was acquired using a 532 nm laser line with a 10-second acquisition time and 10–15 acquisitions. The spectrum exhibits D bands at 1350 cm-1 and 1362 cm-1, corresponding to the k-point phonon breathing mode with A1g symmetry. The D band arises from specific defects such as vacancies and grain boundaries. The G band at 1608 cm-1 corresponds to the E2g phonon of sp2C atoms. The G / D ratio is 1.11. Furthermore, two bands are observed at 2700 and 2900 cm-1, representing the 2D band and the S3 band, respectively. The S3 band is a secondary peak derived from the combination of the DG peaks. Similarly, the 2D band is observed to be broadened, which is attributed to the fact that the prepared graphene contains almost no defective layers. Figures 8 and 9 show thermogravimetric analyses in air and argon (ER-01). Thermogravimetric analyses were performed using synthetic air, approximately 4 mg, from 30°C to 950°C at a heating rate of 10°C / min. One analysis was performed in synthetic air, and the other in argon. The line in Figure 8 shows the thermal decomposition profile of graphene (sample ER-01) in air. The decomposition temperature of graphene begins at approximately 550°C, with complete decomposition occurring at approximately 700°C. The sample is nearly completely decomposed. The line in Figure 9 shows the thermal decomposition profile of graphene (sample ER-01) in argon. The decomposition temperature of graphene begins at approximately 720°C, with complete decomposition occurring at approximately 950°C. 70% remains after this temperature treatment. FIG. 10 shows the C1s spectrum, with peaks at 284 eV, 286 eV, and 288 eV corresponding to C-C, C-O-C, and C-O-C=O bonds, respectively.

[0018] Example 2 - Synthesis of sulfo-graphene (sample ER-02) In Example 2, natural gas was introduced into the reactor along with the aluminum alloy. An inert gas (e.g., nitrogen) was used as a carrier to transport the sulfur-functionalized graphene from the reaction chamber to a collection vessel. The temperature range of the reaction chamber was maintained between 900°C and 1100°C. The total reaction time was 120 minutes. The synthesis variations in temperature / reaction time were as follows: first, 60 minutes at a temperature range of 900°C to 950°C, then increased to approximately 1100°C. The material temperature was held at a plateau between approximately 990°C and 1100°C for 30 minutes. Then, the temperature was held at 900°C to 920°C for 30 minutes. Figures 11A-11H show SEM images of sulfur-graphene flakes obtained from sample ER-02. The sample was dispersed in methanol, sonicated in an ultrasonic bath for 5 minutes, and drop-cast onto a Si / SiO2 wafer. The results showed graphene flakes and nanorods. Figure 12 shows an SEM mapping image of sulfur-graphene flakes obtained from sample ER-02. The sample was dispersed in methanol, sonicated in an ultrasonic bath for 5 minutes, and drop-cast onto a Si / SiO2 wafer. The mapping was obtained according to the initial EDS spectrum of the area obtained from image 13A. Figure 12 shows an image of the mapped area. Figures 13A-13F show TEM images of sulfur-graphene obtained from sample ER-02. These TEM images of sample ER-02 were obtained after dispersion in methanol for 10 minutes using a 10-minute ultrasonic bath. A droplet of the sample was deposited on a nickel TEM grid coated with lacey carbon. Figures 13A-13F show graphene flakes and small carbon / sulfur particles. Figure 14 shows the Raman spectroscopy results of sulfur-graphene for sample ER-02. The Raman spectrum was acquired using a 532 nm laser with a 10-second acquisition time and 10–15 acquisitions. The spectrum exhibits peaks between 161 cm-1 and 434 cm-1, representing contributions from the -SS-, polymerized -SS-, and nanorod (ZnS?) stretching modes (ν). The peak at 654 cm-1 represents the ν of the -CS bond. The D band at 1343 cm-1 corresponds to the shifted A1g symmetry k-point phonon breathing mode. The D band arises from specific defects such as vacancies and grain boundaries. The G band at 1600 cm-1 corresponds to the E2g phonon of sp2C atoms. Additionally, two bands are observed at 2660 and 2890 cm-1, representing the 2D band and the S3 band, respectively. The 2D bands are observed to be broadened, which is attributed to the fact that the prepared graphene contains few layers with defects.

[0019] Example 3 - Synthesis of highly oriented pyrolytic graphite-like material (Sample ER-03) In Example 3, high-density polyethylene (HDPE) was inserted into the reactor along with the aluminum alloy. An inert gas (e.g., nitrogen) was used as a carrier to transport the highly oriented pyrolytic graphite (HOPG)-like material from the reaction chamber to a collection vessel. The temperature range of the reaction chamber was maintained between 900°C and 950°C. Figures 15A-15I show SEM images of highly oriented pyrolytic graphite (HOPG)-like material obtained from sample ER-03. The sample was dispersed in methanol, sonicated in an ultrasonic bath for 5 minutes, and drop-cast onto a Si / SiO2 wafer. The HOPG-like material exhibited graphite flakes embedded in circular graphitic structures. Figures 16, 17, and 18A-18F show SEM mapping images of the HOPG-like material obtained from sample ER-03. The sample was dispersed in methanol, sonicated in an ultrasonic bath for 5 minutes, and drop-cast onto a Si / SiO2 wafer. The mapping was obtained according to the initial EDS spectrum of the area obtained from image 23(a). Figure 16 shows an image of the mapped area. Figure 17 shows the EDS spectrum of the analyzed area. Figures 18A-18C show EDS mappings of carbon (18A), oxygen (18B), and sulfur (18C). Figure 19 shows the Raman spectroscopy results of the HOPG-like material (sample ER-03). The Raman spectrum was acquired using a 532 nm laser line with an acquisition time of 10 seconds and 10–15 acquisitions. The spectrum shows a D band at 1358 cm-1. The D band arises from specific defects such as vacancies and grain boundaries. The G band at 1601 cm-1 corresponds to the E2g phonon of sp2C atoms. Peaks greater than 2500 cm-1 correspond to the spectroscopic signature of a highly oriented pyrolytic graphite (HOPG)-like structure. Figure 20 shows the thermogravimetric analysis of sample ER-03. The thermogravimetric analysis was performed using synthetic air, approximately 4 mg, and a temperature ramp from 30°C to 1000°C at a heating rate of 10°C / min. Figure 20 shows the thermal decomposition profile of sample ER-03 in air. The decomposition temperature of graphene is approximately 555°C. Based on the above data, 96.21% of the sample decomposes at 555°C. Slight decomposition of less than 2% was observed at approximately 200°C, which may be due to instrument calibration or amorphous carbon.

[0020] Additional Embodiments Another contemplated embodiment of the present disclosure is shown in Figure 21. Method 2600 includes a method for producing a carbon material. Step 2610 involves combining a carbon precursor and a catalyst in a controlled, oxygen-free environment, where the reaction is carried out at a temperature ranging from about 600°C to 1400°C. Method 2600 can include multiple variations and embodiments and / or additional and / or alternative steps. An embodiment of a method contemplated in another embodiment of the present disclosure is shown in Figure 23. Method 2800 includes a method for synthesizing carbon. Step 2810 is mixing a feedstock with molten aluminum. Step 2820 is pouring the mixture of molten aluminum and feedstock into a reaction vessel containing additional molten aluminum, where the pouring occurs below the surface of the molten aluminum in the reaction vessel. Step 2830 is reacting the feedstock with the molten aluminum to form one or more carbon-containing products. Method 2800 may include multiple alternative embodiments having additional or alternative steps.

[0021] Abbreviations and Defined Terms To aid in understanding the description set forth herein and the appended claims, several selected terms are defined below. Unless defined otherwise, all technical and scientific terms used herein have the same meaning as commonly understood by one of ordinary skill in the art to which this disclosure pertains. The terms "approximately," "about," and "substantially," as used herein, refer to an amount or condition that is close to a stated amount or condition that still performs a desired function or achieves a desired result. For example, the terms "approximately," "about," and "substantially" can refer to an amount or condition that differs by less than 10%, or less than 5%, or less than 1%, or less than 0.1%, or less than 0.01% from the stated amount or condition.

[0022] Various aspects of the present disclosure, including devices, systems, and methods, may be illustrated with reference to one or more embodiments or implementations that are exemplary in nature. As used herein, the term "exemplary" means "serving as an example, instance, or illustration" and should not necessarily be construed as preferred or advantageous over the embodiments disclosed herein. In addition, references to "implementations" of the present disclosure or embodiments include specific references to one or more embodiments thereof, and vice versa. Such references are intended to provide illustrative examples without limiting the scope of the disclosure, the scope of which is indicated by the appended claims, rather than by the description herein. As used herein, unless otherwise understood or stated, implicitly or explicitly, words denoted in the singular include the corresponding plural, and words denoted in the plural include the corresponding singular. It should also be noted that, as used in this specification and the appended claims, the singular forms "a," "an," and "the" include plural references unless the context clearly dictates otherwise. For example, a reference to the singular (e.g., "a widget") includes one, two, or more references unless otherwise understood or stated, implicitly or explicitly. Similarly, a reference to plural references should be construed as including a single reference and / or plural references unless the content and / or context clearly dictates otherwise. For example, a reference to the plural (e.g., "widgets") does not necessarily require a plurality of such references. Instead, it will be understood that one or more references are contemplated, regardless of the number of references inferred, unless otherwise specified herein.

[0023] References herein to "one embodiment," "an embodiment," "an example embodiment," etc. indicate that the described embodiment may include a particular feature, structure, or characteristic, but not all embodiments necessarily include that particular feature, structure, or characteristic. Moreover, such phrases do not necessarily refer to the same embodiment. Furthermore, when a particular feature, structure, or characteristic is described in connection with an embodiment, it is asserted that it is within the knowledge of one of ordinary skill in the art that such feature, structure, or characteristic also works in connection with other embodiments, whether or not explicitly stated. Although terms such as "first" and "second" may be used herein to describe various elements, it should be understood that these elements are not limited by these terms. These terms are used merely to distinguish one element from another. For example, a first element could be termed a second element, and similarly, a second element could be termed a first element, without departing from the scope of the example embodiments. As used herein, the term "and / or" includes any and all combinations of one or more of the associated listed items. It will be further understood that the terms "comprises," "comprising," "has," "having," "includes," and / or "including," as used herein, specify the presence of stated features, elements, and / or components, etc., but do not exclude the presence or addition of one or more other features, elements, components, and / or combinations thereof.

[0024] Conclusion The present disclosure includes any novel feature or combination of features explicitly disclosed herein, or any generalization thereof. Various modifications and adaptations of the exemplary embodiments of the present disclosure described above will become apparent to those skilled in the art in view of the above description, read in conjunction with the accompanying drawings. However, any and all modifications will still fall within the scope of the non-limiting and exemplary embodiments of the present disclosure. It will further be understood that for any given component or embodiment described herein, any of the possible candidates or alternatives listed for that component may generally be used individually or in combination with each other, unless otherwise implicitly or explicitly understood or stated. It will further be understood that the listing of such candidates or alternatives is merely exemplary and not limiting, unless otherwise implicitly or explicitly understood or stated. Furthermore, unless otherwise indicated, numbers expressing quantities, components, distances, or other measurements used in the specification and claims are to be understood as modified by the term "about," as defined herein. Accordingly, unless otherwise indicated, the numerical parameters set forth in the specification and appended claims are approximations that may vary depending upon the desired properties sought to be obtained by the subject matter described herein. At the very least, and not as an attempt to limit the application of the doctrine of equivalents to the scope of the claims, each numerical parameter should at least be construed in light of the number of reported significant digits and by applying ordinary rounding techniques. Notwithstanding that the numerical ranges and parameters setting forth the broad scope of the subject matter presented herein are approximations, the numerical values ​​set forth in the specific examples are reported as precisely as possible. However, any numerical value inherently contains certain errors necessarily resulting from the standard deviation found in their respective testing measurements. The headings and subheadings used herein are for organizational purposes only and are not intended to be used to limit the scope of the description or claims. The terms and expressions used herein are used as terms of description and not of limitation, and the use of such terms and expressions is not intended to exclude any equivalents of the features shown and described or portions thereof, and it is recognized that various modifications are possible within the scope of the present disclosure. Thus, while the present disclosure has been specifically disclosed in part by certain embodiments and optional additional features, it should be understood that those skilled in the art may employ modifications and variations of the concepts disclosed herein, and such modifications and variations are deemed to be within the scope of the present disclosure.

[0025] It will also be understood that systems, devices, articles of manufacture, kits, methods, and / or processes according to certain embodiments of the present disclosure may include, incorporate, or otherwise include features (e.g., components, members, elements, parts, and / or portions) described in other embodiments disclosed and / or described herein. Accordingly, various features of certain embodiments are compatible with, can be combined with, included in, and / or incorporated into other embodiments of the present disclosure. Accordingly, the disclosure of a particular feature in connection with a particular embodiment of the present disclosure should not be construed as limiting the application or inclusion of that feature to the particular embodiment. Rather, it will be recognized that other embodiments may include such features, members, elements, parts, and / or portions without, of course, departing from the scope of the present disclosure. Furthermore, unless a feature is described as requiring another feature in combination, any feature herein may be combined with any other feature of the same or different embodiments disclosed herein. Moreover, various well-known aspects of example systems, methods, devices, etc. have not been described in particular detail herein to avoid obscuring aspects of the example embodiments. However, such aspects are also contemplated herein. Those skilled in the art will recognize that methods, devices, device elements, materials, procedures, and techniques other than those specifically described herein can be adapted to the practice of the embodiments broadly disclosed herein without undue experimentation. All art-known functional equivalents of the methods, devices, device elements, materials, procedures, and techniques specifically described herein are intended to be encompassed by this disclosure.

[0026] When a group of materials, compositions, components, or compounds is disclosed herein, it is understood that all individual members of that group and all subgroups thereof are separately disclosed. When a Markush group or other classification is used herein, all individual members of that group and all possible combinations and subcombinations of that group are intended to be included individually in the disclosure. The above-described embodiments are by way of example only. Alterations, modifications and variations may be effected in the particular embodiments by those of skill in the art without departing from the scope of the description, which is defined solely by the claims that follow.

Claims

1. 1. A method for producing a carbon material, comprising: mixing a carbon precursor and a catalyst in a controlled, oxygen-free environment, the reaction being carried out in the range of about 600°C to 1400°C; method.

2. The method of claim 1 , wherein the carbon material comprises one or more of graphene, carbon nanostructures, synthetic graphite, sulfur-graphene, and highly oriented pyrolytic graphite.

3. The method of claim 1 wherein the catalyst comprises aluminum.

4. The method of claim 1 further comprising using a secondary catalyst.

5. The method of claim 4 , wherein the secondary catalyst comprises one or more of Mg, Fe, and Co.

6. The method of claim 1 further comprising utilizing the presence of a chalcogenide.

7. The method of claim 6 , wherein the chalcogenide comprises at least one of oxygen, sulfur, selenium, and tellurium.

8. The method of claim 1 further comprising using a carrier gas.

9. The method of claim 8 , wherein the carrier gas comprises at least one of a short chain hydrocarbon, nitrogen, argon, and hydrogen.

10. 10. The method of claim 1 further comprising micronizing, grinding, or jet milling the output product.

11. 1. A method for synthesizing carbon, comprising: mixing a feedstock with molten aluminum; injecting the mixture of molten aluminum and feedstock into a reactor vessel containing additional molten aluminum, said injection occurring below the surface of the molten aluminum in the reactor vessel; reacting the feedstock with the molten aluminum to form one or more carbon-containing products; A method comprising:

12. 12. The method of claim 11, wherein the one or more carbon materials comprise one or more of graphene, carbon nanostructures, synthetic graphite, sulfur-graphene, and highly oriented pyrolytic graphite.

13. The method of claim 11 further comprising using a secondary catalyst.

14. The method of claim 11 further comprising utilizing the presence of a chalcogenide.

15. 12. The method of claim 11, wherein the method avoids the use of oxygen.

16. The method of claim 11 further comprising using a carrier gas.

17. 1. A reaction vessel for reacting a carbon precursor with molten metal, comprising: a reactor vessel wall; a refractory material lining the inside of the reactor vessel wall; a cooling plate attached to the outside of the reactor vessel wall, the cooling plate forming a flow path for a cooling liquid between the cooling plate and the reactor vessel wall; an aluminum supply line running to the reactor vessel wall; an injection line through the reactor vessel wall and having an outlet within the reactor vessel, the injection line configured to deliver the carbon precursor to the reactor vessel; one or more withdrawal lines passing through the reactor vessel wall and configured to withdraw one or more output products; A reaction vessel comprising:

18. 18. The reaction vessel of claim 17, wherein the outlet of the injection line is positioned to introduce the carbon precursor into the reaction vessel below a top surface of the molten metal, thereby mixing the carbon precursor with the molten metal and causing the carbon precursor to react with the molten metal to produce a liquefied product.

19. 18. The reactor vessel of claim 17, wherein the liquefied product separates from the molten metal by settling to the bottom of the reactor vessel.

20. 18. The reaction vessel of claim 17, wherein the one or more recovery lines comprise first and section recovery lines, wherein a lighter density first component is removed using the first recovery line and a heavier density second component is removed using the second recovery line.

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