Systems and methods for electrical processing - Patents.com
Patent Information
- Application Number
- JP2024520921
- Authority / Receiving Office
- JP · JP
- Patent Type
- Applications
- Current Assignee / Owner
- Priority Date
- 2022-09-08
- Filing Date
- 2022-09-30
- Publication Date
- 2025-10-22
AI Technical Summary
Existing processes for producing carbonaceous materials and hydrogen are inefficient and lack effectiveness in terms of energy and environmental performance.
A method involving the heating of hydrocarbons with a plasma generator at pressures above atmospheric pressure, using AC or DC electrodes, to produce hydrogen and carbonaceous materials in a single-step, oxygen-free environment, utilizing a once-through process with equipment like heat exchangers and solids handling systems.
This method enhances the efficiency and yield of hydrogen and carbonaceous material production, achieving higher yields and purities while reducing energy consumption and environmental impact.
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Abstract
Description
[Technical field]
[0001] cross reference This application claims the benefit of U.S. Provisional Application No. 63 / 253,996, filed October 8, 2021, U.S. Provisional Application No. 63 / 375,024, filed September 8, 2022, U.S. Provisional Application No. 63 / 298,912, filed January 12, 2022, and U.S. Provisional Application No. 63 / 350,801, filed June 9, 2022, each of which is incorporated by reference in its entirety herein. [Background technology]
[0002] Carbonaceous materials and / or hydrogen can be produced by a variety of chemical processes, the performance, energy supply, and environmental performance associated with such chemical processes have evolved over time. Summary of the Invention
[0003] The present disclosure recognizes the need for more efficient and effective processes for producing, for example, carbonaceous materials and / or hydrogen.
[0004] The present disclosure provides a processing method that includes, for example, producing hydrogen by heating a hydrocarbon with a plasma generator at a pressure greater than atmospheric pressure. The method may further include adding a hydrocarbon to a plasma generator. The plasma generator may include AC or DC electrodes. The method may further include producing a carbonaceous material. The carbonaceous material may include carbon particles. The method may further include sequentially producing hydrogen and a carbonaceous material. The hydrocarbon may be a gas, natural gas, or may include natural gas. The method may further include heating a hydrocarbon to produce hydrogen in a single chamber. The method may further include producing hydrogen and a carbonaceous material in a once-through single-stage process. The method is performed at a pressure of about 2 bar or greater. The method is performed at a pressure of about 5 bar or greater. The method is performed at a pressure of about 10 bar or greater.
[0005] The present disclosure also provides a process method comprising producing hydrogen in a substantially inert or substantially oxygen-free environment or atmosphere, for example, by heating a hydrocarbon with electrical energy at a pressure above atmospheric pressure. The method may further comprise producing a carbonaceous material. The carbonaceous material may comprise carbon particles. The method may further comprise continuously producing hydrogen and a carbonaceous material. The hydrocarbon may be gas, natural gas, or may comprise natural gas. The method may further comprise directly heating the hydrocarbon with electrical energy. The hydrogen may be produced in a refractory-lined reactor. The method may further comprise heating the hydrocarbon to produce hydrogen in a single chamber. The method may further comprise producing the hydrogen and the carbonaceous material in a once-through, single-stage process. The method may further comprise removing hydrogen from the hydrogen using electrical energy. The method is performed at a pressure of about 2 bar or greater. The method is performed at a pressure of about 5 bar or greater. The method is performed at a pressure of about 10 bar or greater. The method may further include using a heat exchanger, a filter, and solids handling equipment. The solids handling equipment may include a cooled solids carbon collection screw conveyor, an airlock and purge system, a pneumatic conveying system, a mechanical conveying system, a classifying mill, and a product storage vessel. The method may further include generating hydrogen in a substantially oxygen free environment or atmosphere. The method may further include generating hydrogen in a substantially inert environment or atmosphere.
[0006] The present disclosure also provides a method of producing hydrogen in a substantially inert or substantially oxygen-free environment or atmosphere, for example, by directly heating a hydrocarbon with electrical energy. The hydrocarbon may be or include a gas, natural gas. The method may further include producing a carbonaceous material. The carbonaceous material may include carbon particles. The method may further include producing hydrogen and a carbonaceous material sequentially. The method may further include generating a plasma. The plasma may be generated using AC electrodes. The plasma may be generated using DC electrodes. The method may further include producing hydrogen in an environment or atmosphere containing less than about 2% molecular oxygen by volume or molar. The method may further include heating a hydrocarbon to produce hydrogen in a single chamber. The method may further include producing hydrogen and a carbonaceous material in a once-through, single-step process.
[0007] In another aspect, the disclosure provides a method of producing carbon particles in a reactor, the method comprising: (a) generating a plasma in the reactor using one or more electrodes; and (b) injecting hydrocarbons into the reactor through one or more injectors such that the hydrocarbons contact the plasma, thereby producing carbon particles, wherein the reactor is operated at a pressure of about 1.5 bar or greater.
[0008] In some embodiments, the one or more electrodes include an AC electrode. In some embodiments, the one or more electrodes include a DC electrode. In some embodiments, the method further includes producing hydrogen. In some embodiments, the method further includes continuously producing hydrogen and carbon particles. In some embodiments, the method further includes producing hydrogen and carbon particles in a once-through, single-stage process. In some embodiments, the hydrocarbon is a gas. In some embodiments, the hydrocarbon includes natural gas. In some embodiments, the hydrocarbon is heated upon contact with the plasma. In some embodiments, the carbon particles have a smaller surface area than carbon particles formed in the reactor when operated at a pressure less than about 1.5 bar. In some embodiments, the carbon particles have about 90% of the surface area compared to carbon particles formed in the reactor when operated at a pressure of about 1 bar. In some embodiments, the reactor is operated at a pressure of about 5 bar or more. In some embodiments, the carbon particles have a smaller surface area than carbon particles formed in the reactor when operated at a pressure less than about 5 bar. In some embodiments, the carbon particles have about 60% of the surface area compared to carbon particles formed in the reactor when operated at a pressure of about 1 bar. In some embodiments, the reactor is operated at a pressure of about 10 bar or more. In some embodiments, the carbon particles have a smaller surface area than carbon particles formed in the reactor when operated at a pressure less than about 10 bar. In some embodiments, the carbon particles have about 35% of the surface area compared to carbon particles formed in the reactor when operated at a pressure of about 1 bar. In some embodiments, the reactor is operated at a pressure of about 20 bar or more. In some embodiments, the carbon particles have a smaller surface area than carbon particles formed in the reactor when operated at a pressure less than about 20 bar. In some embodiments, the reactor is operated at a pressure of about 30 bar or more. In some embodiments, the carbon particles have a smaller surface area than carbon particles formed in the reactor when operated at a pressure less than about 30 bar. In some embodiments, the method further comprises increasing the surface area of the carbon particles using one or more additives.In some embodiments, the one or more additives include a hydrocarbon gas. In some embodiments, the one or more additives include silicon. In some embodiments, the one or more additives include an aromatic additive. In some embodiments, the reactor is an oxygen-free environment. In some embodiments, the reactor includes less than about 2% molecular oxygen by volume or molar. In some embodiments, the yield of carbon particles in the reactor is higher than the yield of carbon particles formed in the reactor when operated at a pressure of about 1 bar. In some embodiments, the carbon particles are produced in a yield of greater than 75%. In some embodiments, the carbon particles are produced in a yield of greater than 85%. In some embodiments, the carbon particles are produced in a yield of greater than 90%. In some embodiments, the carbon particles are produced in a yield of greater than 99%. In some embodiments, the yield of carbon particles in the reactor is higher than the yield of carbon particles formed in a reactor of the same size as the reactor when operated at a pressure of less than 1.5 bar.
[0009] In another aspect, the disclosure provides a method of producing hydrogen in a reactor, the method comprising: (a) generating a plasma in the reactor using one or more electrodes; and (b) injecting hydrocarbons into the reactor through one or more injectors such that the hydrocarbons contact the plasma, thereby producing hydrogen, wherein the reactor is operated at a pressure of about 1.5 bar or greater.
[0010] In some embodiments, the one or more electrodes include an AC electrode. In some embodiments, the one or more electrodes include a DC electrode. In some embodiments, the method further includes producing carbon particles. In some embodiments, the method further includes continuously producing hydrogen and carbon particles. In some embodiments, the method further includes producing hydrogen and carbon particles in a once-through, single-stage process. In some embodiments, the hydrocarbon is a gas. In some embodiments, the hydrocarbon includes natural gas. In some embodiments, the hydrocarbon is heated upon contact with the plasma. In some embodiments, the reactor is operated at a pressure of about 5 bar or greater. In some embodiments, the reactor is operated at a pressure of about 10 bar or greater. In some embodiments, the reactor is operated at a pressure of about 20 bar or greater. In some embodiments, the reactor is operated at a pressure of about 30 bar or greater. In some embodiments, the reactor is an oxygen-free environment. In some embodiments, the reactor includes less than about 2% molecular oxygen by volume or mole.
[0011] In another aspect, the disclosure provides a method of producing carbon particles in a reactor, the method comprising: (a) generating a plasma in the reactor using one or more electrodes; and (b) injecting hydrocarbons into the reactor through one or more injectors, thereby producing carbon particles, wherein the reactor is operated at a pressure of about 1.5 bar or greater.
[0012] In some embodiments, the one or more electrodes include an AC electrode. In some embodiments, the one or more electrodes include a DC electrode. In some embodiments, the method further includes producing hydrogen. In some embodiments, the method further includes continuously producing hydrogen and carbon particles. In some embodiments, the method further includes producing hydrogen and carbon particles in a once-through, single-stage process. In some embodiments, the hydrocarbon is a gas. In some embodiments, the hydrocarbon includes natural gas. In some embodiments, the hydrocarbon is heated upon contact with the plasma. In some embodiments, the carbon particles have a smaller surface area than carbon particles formed in the reactor when operated at a pressure less than about 1.5 bar. In some embodiments, the carbon particles have about 90% of the surface area compared to carbon particles formed in the reactor when operated at a pressure of about 1 bar. In some embodiments, the reactor is operated at a pressure of about 5 bar or more. In some embodiments, the carbon particles have a smaller surface area than carbon particles formed in the reactor when operated at a pressure less than about 5 bar. In some embodiments, the carbon particles have about 60% of the surface area compared to carbon particles formed in the reactor when operated at a pressure of about 1 bar. In some embodiments, the reactor is operated at a pressure of about 10 bar or more. In some embodiments, the carbon particles have a smaller surface area than carbon particles formed in the reactor when operated at a pressure less than about 10 bar. In some embodiments, the carbon particles have about 35% of the surface area compared to carbon particles formed in the reactor when operated at a pressure of about 1 bar. In some embodiments, the reactor is operated at a pressure of about 20 bar or more. In some embodiments, the carbon particles have a smaller surface area than carbon particles formed in the reactor when operated at a pressure less than about 20 bar. In some embodiments, the reactor is operated at a pressure of about 30 bar or more. In some embodiments, the carbon particles have a smaller surface area than carbon particles formed in the reactor when operated at a pressure less than about 30 bar. In some embodiments, the method further comprises increasing the surface area of the carbon particles using one or more additives.In some embodiments, the one or more additives include a hydrocarbon gas. In some embodiments, the one or more additives include silicon. In some embodiments, the one or more additives include an aromatic additive. In some embodiments, the reactor is an oxygen-free environment. In some embodiments, the reactor includes less than about 2% molecular oxygen by volume or molar. In some embodiments, the yield of carbon particles in the reactor is higher than the yield of carbon particles formed in the reactor when operated at a pressure of about 1 bar. In some embodiments, the carbon particles are produced in a yield of greater than 75%. In some embodiments, the carbon particles are produced in a yield of greater than 85%. In some embodiments, the carbon particles are produced in a yield of greater than 90%. In some embodiments, the carbon particles are produced in a yield of greater than 99%. In some embodiments, the yield of carbon particles in the reactor is higher than the yield of carbon particles formed in a reactor of the same size as the reactor when operated at a pressure of less than 1.5 bar.
[0013] In another aspect, the disclosure provides a method of producing hydrogen in a reactor, the method comprising: (a) generating a plasma in the reactor using one or more electrodes; and (b) injecting hydrocarbons into the reactor through one or more injectors, thereby producing hydrogen, wherein the reactor is operated at a pressure of about 1.5 bar or greater.
[0014] In some embodiments, the one or more electrodes include an AC electrode. In some embodiments, the one or more electrodes include a DC electrode. In some embodiments, the method further includes producing carbon particles. In some embodiments, the method further includes continuously producing hydrogen and carbon particles. In some embodiments, the method further includes producing hydrogen and carbon particles in a once-through, single-stage process. In some embodiments, the hydrocarbon is a gas. In some embodiments, the hydrocarbon includes natural gas. In some embodiments, the hydrocarbon is heated upon contact with the plasma. In some embodiments, the reactor is operated at a pressure of about 5 bar or more. In some embodiments, the reactor is operated at a pressure of about 10 bar or more. In some embodiments, the reactor is operated at a pressure of about 20 bar or more. In some embodiments, the reactor is operated at a pressure of about 30 bar or more. In some embodiments, the reactor is an oxygen-free environment. In some embodiments, the reactor includes less than about 2% molecular oxygen by volume or mole. In some embodiments, the hydrocarbon is injected adjacent to the one or more electrodes. In some embodiments, the hydrocarbon is injected within 500 millimeters (mm) of one or more electrodes. In some embodiments, the plasma contains at least a portion of the hydrocarbon. In some embodiments, the hydrocarbon contacts the plasma after the injecting step in (b). In some embodiments, each of the one or more electrodes comprises an electrode tip, and the one or more electrode tips are positioned in a single plane within the reactor. In some embodiments, the hydrocarbon is injected into the reactor upstream of the single plane of the one or more electrode tips. In some embodiments, the hydrocarbon is injected into the reactor at the single plane of the one or more electrode tips. In some embodiments, the hydrocarbon is injected into the reactor downstream of the single plane of the one or more electrode tips. In some embodiments, the pressure at the injection tip of the one or more injectors is greater than 1.5 bar. In some embodiments, the operating pressure of the reactor is within 10% of the pressure at the injector tip. In some embodiments, more than 30% of the carbon particles are carbon particles having an equivalent spherical diameter of less than about 2 micrometers.In some embodiments, more than 30% of the carbon particles are carbonaceous nanoparticles. In some embodiments, more than 90% of the carbon injected into the reactor forms either carbon particles having an equivalent spherical diameter of less than about 2 micrometers or carbon particles having an equivalent spherical diameter of less than about 2 micrometers. In some embodiments, the combination of larger carbon particles and carbon particles comprises more than 98% carbon. In some embodiments, the hydrogen produced has a purity of more than 99.9%. In some embodiments, the method further comprises directing the hydrogen produced to a purification system without compressing or repressurizing the hydrogen produced. In some embodiments, the method further comprises isolating the carbon particles using a pressure lock system to remove at least a portion of the hydrogen produced and reducing the atmosphere surrounding the carbon particles to less than 1.5 bar. In some embodiments, the carbon particles comprise a carbon-14 ratio greater than the carbon-14 ratio of carbon particles produced using a fossil fuel hydrocarbon feedstock. In some embodiments, each of the one or more electrodes has a mass of more than 10 kg. In some embodiments, more than 3 tons / hour of carbon particles are produced. In some embodiments, more than 1 ton / hour of hydrogen is produced. In some embodiments, the method further comprises adding a sheath gas to the reactor. In some embodiments, adding the sheath gas increases the yield of carbonaceous nanoparticles compared to methods without adding the sheath gas. In some embodiments, the wear rate of the one or more electrodes is less than 10 kg per electrode per ton of carbon particles produced. In some embodiments, the hydrocarbons are injected adjacent to the one or more electrodes. In some embodiments, the hydrocarbons are injected within 500 millimeters (mm) of the one or more electrodes. In some embodiments, the plasma comprises at least a portion of the hydrocarbons. In some embodiments, the hydrocarbons contact the plasma after the injection step in (b). In some embodiments, each of the one or more electrodes comprises an electrode tip, and the one or more electrode tips are positioned in a single plane within the reactor. In some embodiments, the hydrocarbons are injected into the reactor upstream of the single plane of the one or more electrode tips.In some embodiments, the hydrocarbon is injected into the reactor at a single plane of one or more electrode tips. In some embodiments, the hydrocarbon is injected into the reactor downstream of a single plane of one or more electrode tips. In some embodiments, the pressure at the injection tip of the one or more injectors is greater than 3.3 bar. In some embodiments, the operating pressure of the reactor is within 10% of the pressure at the injector tip. In some embodiments, the hydrogen produced has a purity of greater than 99.9%. In some embodiments, the method further comprises directing the hydrogen produced to a purification system without compressing or repressurizing the hydrogen produced. In some embodiments, each of the one or more electrodes has a mass of greater than 20 kg. In some embodiments, greater than 1 ton / hour of hydrogen is produced. In some embodiments, the method further comprises adding a sheath gas to the reactor. In some embodiments, the hydrocarbon comprises a liquid hydrocarbon. In some embodiments, the hydrocarbon is used as a plasma gas to generate the plasma.
[0015] These additional embodiments are described further below.
[0016] INCORPORATION BY REFERENCE All publications, patents, and patent applications mentioned in this specification are herein incorporated by reference to the same extent as if each individual publication, patent, or patent application was specifically and individually indicated to be incorporated by reference. To the extent that the publications and patents or patent applications incorporated by reference conflict with a disclosure contained in the specification, the specification is intended to supersede and / or override any such conflicting material.
[0017] The novel features of the invention are set forth with particularity in the appended claims. A better understanding of the features and advantages of the present invention will be obtained by reference to the following detailed description that sets forth illustrative embodiments, in which the principles of the invention are utilized, and the accompanying drawings or figures (also referred to herein as "FIG." and "FIGs."), in which: [Brief description of the drawings]
[0018] [Figure 1] 1 illustrates an example of a system according to the present disclosure. [Diagram 2] 1 shows a schematic diagram of an example of an apparatus according to the present disclosure. [Diagram 3] 1 shows a schematic diagram of another example of an apparatus according to the present disclosure. [Figure 4] 1 shows a schematic diagram of another example of an apparatus according to the present disclosure. [Diagram 5] 1 illustrates a flow chart of a process for forming carbon particles in a reactor, according to some embodiments. [Figure 6] 1 shows a flow chart of a process for producing hydrogen in a reactor, according to some embodiments. [Figure 7] 1 is a plot of an example of a range of reactor pressure versus normalized surface area measurements according to an embodiment. [Figure 8] 1 is a plot of a demonstration example of increasing reactor yield with increasing reactor pressure, according to an embodiment. [Figure 9] 1 illustrates a computer system that is programmed or otherwise configured to carry out the methods provided herein. [Figure 10] 1 is an example of a high pressure degasser according to some embodiments. DETAILED DESCRIPTION OF THE PREFERRED EMBODIMENTS
[0019] The details shown in this specification are by way of example and merely for the purpose of illustrative description of various embodiments of the present invention, and are presented in order to provide what is believed to be the most useful and readily understood explanation of the principles and conceptual aspects of the present invention. In this regard, no attempt has been made to show the details of the present invention in more detail than is necessary for a fundamental understanding of the invention, and the description will make clear to those skilled in the art how some forms of the invention may be embodied in practice.
[0020] The present invention will now be described with reference to more detailed embodiments. However, the present invention may be embodied in different forms and should not be construed as limited to the embodiments set forth herein. Rather, these embodiments are provided so that this disclosure will be thorough and complete, and will fully convey the scope of the invention to those skilled in the art.
[0021] Unless otherwise defined, all technical and scientific terms used herein have the same meaning as commonly understood by those skilled in the art to which this invention belongs. The terms used in the description of the invention herein are intended to describe specific embodiments only and are not intended to limit the invention. As used in the description of the invention and the appended claims, the singular forms "a", "an" and "the" are intended to include the plural forms unless the context clearly indicates otherwise. All publications, patent applications, patents, and other references mentioned herein are expressly incorporated by reference in their entirety.
[0022] Unless otherwise indicated, all numbers expressing quantities of ingredients, reaction conditions, and the like used in the specification and claims are to be understood as being modified in all instances by the term "about." Accordingly, unless indicated to the contrary, the numerical parameters set forth in the following specification and appended claims are approximations that may vary depending upon the properties sought to be obtained by the present invention. 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 be construed in light of the number of significant digits and ordinary rounding approaches.
[0023] Notwithstanding that the numerical ranges and parameters setting forth the broad scope of the invention are approximations, the numerical values set forth in the specific examples are reported as precisely as possible. Any numerical value, however, inherently contains certain errors necessarily resulting from the standard deviation found in their respective testing measurements. Every numerical range given throughout this specification includes every narrower numerical range that falls within such broader numerical range, as if such narrower numerical ranges were all expressly written herein.
[0024] Additional advantages of the present invention will be set forth in part in the description which follows, and in part will be obvious from the description, or may be learned by the practice of the invention. It is to be understood that both the foregoing general description and the following detailed description are exemplary and explanatory only and are not restrictive of the invention as claimed. It is to be understood that different aspects of the present invention can be realized individually, collectively, or in combination with one another.
[0025] Whenever the terms "at least," "greater than," or "greater than or equal to" precede the first number in a series of two or more numbers, the terms "at least," "greater than," or "greater than or equal to" apply to each number in the series. For example, 1, 2, or 3 or more is equivalent to 1 or more, 2 or more, or 3 or more.
[0026] Whenever the terms "not greater than," "less than," or "equal to or less than" precede the first number in a series of two or more numbers, the term "not greater than," "less than," or "equal to or less than" applies to each number in the series. For example, 3, 2, or 1 or less is equivalent to 3 or less, 2 or less, and 1 or less.
[0027] Certain embodiments of the invention herein contemplate numerical ranges. When a range exists, the range includes the end points of the range. Furthermore, all subranges and values within the range exist as if explicitly written out. The term "about" or "approximately" can mean within an acceptable error range for a particular value, which depends in part on how the value is measured or determined, for example, on the limitations of the measurement system. For example, "about" can mean within one standard deviation or more than one standard deviation, as is customary in the art. Alternatively, "about" can mean a range of up to 20%, up to 10%, up to 5%, or up to 1% of a given value. When a particular value is described in the present application and claims, unless otherwise stated, the term "about" can be assumed to mean within an acceptable error range for the particular value.
[0028] The present disclosure provides systems and methods for affecting chemical changes. Affecting such chemical changes may include, for example, forming carbonaceous materials and / or hydrogen using the systems and methods of the present disclosure. The carbonaceous materials may be solid. The carbonaceous materials may include or be, for example, carbon particles, carbon-containing compounds, or combinations thereof. The carbonaceous materials may include, for example, carbon black. The systems (e.g., apparatus) and methods of the present disclosure, and processes implemented using the systems and methods herein, may enable, for example, continuous production of carbonaceous materials and / or hydrogen. The process may include converting a feedstock (e.g., one or more hydrocarbons). The systems and methods described herein may include rapidly heating one or more hydrocarbons to, for example, form carbonaceous materials and / or hydrogen. For example, one or more hydrocarbons may be rapidly heated to form carbon particles and / or hydrogen. Hydrogen may refer to most hydrogen (H2) in some cases. For example, a portion of this hydrogen may also contain methane (e.g., unused methane) and / or various other hydrocarbons (e.g., ethane, propane, ethylene, acetylene, benzene, toluene, polycyclic aromatic hydrocarbons (PAHs), such as naphthalene, etc.).
[0029] The present disclosure provides examples of such systems and methods, including, for example, the use of plasma technology in the pyrolysis (e.g., pyrolytic dehydrogenation) of natural gas into carbonaceous materials (e.g., solid carbonaceous materials, e.g., carbon particles) and / or hydrogen. Pyrolysis (e.g., pyrolytic dehydrogenation) may refer to the thermal decomposition of materials at high temperatures (e.g., temperatures greater than about 800°C) in an inert or oxygen-free environment or atmosphere. The reactor temperature can be increased to increase the conversion of the feedstock to carbon particles and / or hydrogen. The reactor temperature can be increased to selectivity between hydrogen and carbon particles. The reactor temperature can be adjusted to increase or decrease the surface area of the carbon particles. Increasing the temperature can increase the kinetic rate of feedstock decomposition, as well as intermediate operations that can produce the formation of carbon particles and hydrogen. Increasing the reactor temperature can increase the aging rate of the carbon particles and reduce contamination of the reactor walls. This may be because the time it takes for the carbon particles to become chemically inert is reduced.
[0030] The process according to the present disclosure can include heating one or more gases with electrical energy (e.g., from a DC or AC power source). Descriptions herein of heating a gas or heating one or more gases can equally apply to heating a gaseous mixture (e.g., at least 50% (by volume) gaseous) having a corresponding composition. The gaseous mixture may include, for example, a mixture of individual gases and / or liquids, or a mixture of individual gas-liquid mixtures. Any description of a gas herein can equally apply to a liquid or gas-liquid mixture having a corresponding composition, at least in some configurations. The one or more gases can be heated by an electric arc. The one or more gases can be heated by Joule heating (e.g., resistive heating, inductive heating, or a combination thereof). The one or more gases can be heated by Joule heating and an electric arc (e.g., downstream of the Joule heating). The one or more gases can be heated by heat exchange, Joule heating, an electric arc, or any combination thereof. The one or more gases can be heated by heat exchange, Joule heating, combustion, or any combination thereof. At least one of the one or more gases may comprise a hydrocarbon. The one or more gases may comprise a feedstock. The one or more gases may comprise the feedstock alone or in combination with other gases (which may be referred to herein as "process gases", either alone or in combination with other gases that are not heated). The one or more gases may comprise a feedstock and at least one process gas. Individual gases within the one or more gases may be fed (e.g., to a reactor) separately or in various combinations. At least a subset of the one or more gases may be preheated. For example, the hydrocarbon (e.g., feedstock) may be preheated (e.g., from a temperature of about 25°C) to a temperature of about 100°C to about 800°C before being fed to the thermal generator. The process may include heating at least a subset of the one or more gases (e.g., feedstock) at suitable reaction conditions (e.g., in a reactor). The carbonaceous material and / or hydrogen may be produced in a substantially inert or substantially oxygen-free environment or atmosphere.At least a subset of the one or more gases (e.g., feedstock) may be heated in a substantially oxygen-free environment or atmosphere. A substantially oxygen-free environment or atmosphere may, for example, contain less than about 10%, 9%, 8%, 7%, 6%, 5%, 4%, 3%, 2%, or 1% molecular oxygen by volume or mole. A substantially oxygen-free environment or atmosphere may, for example, contain less than about 10%, 9%, 8%, 7%, 6%, 5%, 4%, 3%, 2%, or 1% atomic oxygen by volume or mole. Heating may affect the removal of hydrogen from the feedstock. A feedstock (e.g., one or more hydrocarbons) may be decomposed such that at least about 80% moles of hydrogen initially chemically bonded to the hydrocarbons by covalent bonds may be homoatomically bonded as diatomic hydrogen. A homoatomic bond may refer to a bond between two atoms that are the same (e.g., as in diatomic hydrogen (H2)). CH may be a heteroatomic bond. Hydrocarbons may be heteroatomic bonds CH to homoatomic bonds HH and CC. The reaction products may include, for example, a gaseous and solid effluent stream exiting the reactor. The effluent stream including the reaction products may be cooled. The reaction products may be at least partially separated (e.g., after cooling). For example, the solid carbonaceous material may be at least partially separated from other (e.g., gaseous) reaction products.
[0031] The systems described herein may include a plasma generator. The plasma generator may utilize a gas or gas mixture (e.g., at least 50% gaseous by volume). The plasma generator may utilize a gas or gaseous mixture (e.g., at least 50% gaseous by volume) in which the gas is reactive and corrosive in the plasma state. The plasma generator may be a plasma torch. The systems described herein may include a plasma generator powered by a DC or AC power source. The gas or gas mixture may be directly fed into a zone in which an electric discharge generated by a DC or AC source is sustained. The plasma may have a composition as described elsewhere herein (e.g., with respect to the composition of one or more gases). The plasma may be generated using arc heating. The plasma may be generated using induction heating. The plasma may be generated using DC electrodes. The plasma may be generated using AC electrodes. For example, multiple (e.g., three or more) AC electrodes may be used (e.g., with the advantages of more efficient energy consumption as well as reduced heat load at the electrode surface).
[0032] FIG. 1 illustrates an example of a system 100 according to the present disclosure. The system may include a heat generator (e.g., plasma generator) 101. The heat generator 101 may heat at least a subset of one or more gases (e.g., feedstock) at suitable reaction conditions in a reactor (or furnace) 102 to affect removal of hydrogen from the feedstock. The reactor 102 may house the heat generator (e.g., plasma generator) 101. Heating (e.g., electrical heating such as plasma heating) and reaction may be performed in one chamber (also referred to herein as a "single chamber," "single stage reactor," or "single stage process"). The reactor 102 may include one or more constant diameter regions / sections, one or more converging regions / sections, one or more diverging regions / sections, one or more additional components, or any combination thereof. Such regions / sections, and / or additional components may be combined in various ways to perform heating and reaction according to the present disclosure. Such embodiments may include, but are not limited to, configurations as described in connection with the schematics of FIGS. 2, 3, and 4. For example, the reactor may have a substantially constant diameter (e.g., at least about 70%, 80%, 90%, 95% or 99% of the length of the reactor may be of constant diameter). At least one or more subsets of gases (e.g., feedstocks) may be added to the heat generator 101. The feedstocks (e.g., one or more hydrocarbons) may begin to crack and decompose before being fully converted to solid carbonaceous materials. Heat may be (e.g., can be) provided by latent radiation heat from the walls of the reactor. This may occur by heating the walls (or a portion thereof) via externally supplied energy or by heating the walls (or a portion thereof) from heated gases within the reactor. The reaction products may be cooled after production. A quench (e.g., including process gas) may be used to cool the reaction products. For example, a quench including most of the hydrogen gas may be used. The quench may be added (e.g., by injection) into the reactor 102. A heat exchanger 103 (eg, connected to the reactor 102) can cool an effluent stream containing the reaction products.In the heat exchanger, the gaseous reaction products are exposed to a large surface area and may therefore be cooled while the solid carbonaceous material may be simultaneously transported through the process. The solid carbonaceous material may pass through a filter (e.g., a main filter) 104 (e.g., connected to the heat exchanger 103). The filter may, for example, pass more than 50% of the gaseous reaction products and capture substantially all of the solid carbonaceous material on the filter. For example, at least about 98% (by weight) of the solid carbonaceous material may be captured on the filter. The gaseous reaction products may be provided or coupled to one or more applications, may be recycled back to the reactor (e.g., as process gas), or any combination thereof. The solid carbonaceous material with residual gaseous reaction products may pass through a degasser (e.g., a degasser chamber or device) 105 (e.g., connected to the filter 104) where the amount of combustible gas is reduced (e.g., to less than about 10% (by volume)). The solid carbonaceous material may then pass through a back end 106. The backend equipment 106 may include, for example, one or more of a pelletizer (e.g., connected to the degasser 105), a binder mix tank (e.g., connected to a pelletizer), a dryer (e.g., connected to a pelletizer), and / or a bagger, as non-limiting examples of components or unit operations. For example, the solid carbonaceous material may be dried (e.g., carbon black) pelletized in a pelletizer and dried (e.g., mixed with water along with a binder and then formed into pellets, followed by removal of most of the water in the dryer). The solid carbonaceous material may also pass through a classifier, hammer mill, and / or other size reduction equipment (e.g., to reduce the percentage of grit in the product).Non-limiting examples of other components or unit operations include one or more of a conveying process or conveying unit, a purge filter unit (e.g., capable of filtering solid carbonaceous material from vapors exhausted from a dryer), a dust filter unit (e.g., capable of collecting dust from other equipment), other process filters, other hydrogen / tail gas removal units, cyclones, other bulk separation (e.g., solids / gas separation) units, off-quality product blending units, and the like (e.g., other components or unit operations described elsewhere herein). Components or unit operations can be added or removed as needed. For example, system 100 can include at least one or more heat exchangers 103, one or more filters 104, and a back end 106 comprising solid handling equipment. The solid handling equipment can include, for example, a cooled solid carbon collection screw conveyor, an airlock and purge system, a pneumatic conveying system, a mechanical conveying system (e.g., a conveyor belt auger or elevator), a classifying mill, and a product storage vessel. The carbon particles can be collected at a single location (e.g., all carbon particles can be collected at one location). The carbon particles may be collected at multiple locations (e.g., a portion of the carbon particles can be collected at a first location and a second portion of the carbon particles can be collected at a second location). In some cases, when the carbon particles are collected at multiple locations, the first of the multiple locations can be a catch pot. The catch pot can be configured to collect larger carbon particles that are not carried through the system (e.g., due to gravity). In some cases, the catch pot can operate using a pressure lock dump device (e.g., the high pressure degasser of FIG. 10). In some cases, when the carbon particles are collected at multiple locations, an apparatus such as that of FIG. 10 can be used to collect the smaller carbon particles. The apparatus of FIG. 10 can be located downstream of the catch pot. In some cases, the first catch pot can be located below the reactor (e.g., directly below, close to directly below, near directly below). In some cases, a second particle collector (e.g., a catch pot, etc.) can be located downstream of the reactor.The second particle collector can be configured to collect smaller carbon particles carried by the reactor effluent stream. The first catch pot can be configured to capture larger carbon particles as described elsewhere herein (e.g., carbon particles having a spherical equivalent diameter greater than about 2 micrometers). The second particle collector may be configured to capture carbon particles as described elsewhere herein (e.g., carbon particles having a spherical equivalent diameter up to about 2 micrometers).
[0033] Other examples of separation units or hydrogen / tail gas removal units include, but are not limited to, pressure swing adsorption units, cryogenic separation units, molecular sieves, and the like, or any combination thereof. Pressure swing adsorption (PSA) units may be configured to separate and / or purify components from a gas stream (e.g., components from a gas stream produced by a reactor as described elsewhere herein). PSA units may include the use of adsorption and the properties of different components of a gas mixture (e.g., molecular size, dipole moment, and the like) to selectively pass components of the mixture. For example, a PSA unit may be used to separate hydrogen from a reactor gas mixture. In this example, the PSA unit may separate hydrogen using small size hydrogen by passing the gas mixture over a porous bed (e.g., a bed of porous zeolite) that may act as a sieve. In this example, hydrogen may pass through the sieve, while larger species in the gas mixture are filtered out by being trapped in the sieve. In this example, the sieve may be saturated with the larger gas, at which point the bed may be removed and regenerated by removal of the larger gas species. Multiple PSA units may be used in parallel or series. For example, multiple PSA units can be set up in parallel to allow for continuous processing of gas while a subset of the PSA units is being regenerated. The PSA units can operate at pressures of at least about 1, 5, 10, 11, 12, 13, 14, 15, 16, 17, 18, 19, 20, 21, 22, 23, 24, 25, 26, 27, 28, 29, 30, or more barg. The PSA units can operate at pressures of up to about 30, 29, 28, 27, 26, 25, 24, 23, 22, 21, 20, 19, 18, 17, 16, 15, 14, 13, 12, 11, 10, 5, or fewer barg. The PSA units can operate at pressures within a range defined by any two of the progression values. For example, the PSA units can operate at pressures of about 13 to about 24 barg.The PSA unit can operate at gas inlet temperatures of at least about -50, -45, -40, -35, -30, -25, -20, -15, -10, -5, 0, 5, 10, 15, 20, 25, 30, 35, 40, 45, 50, 55, 60, 65, 70 degrees Celsius or more. The PSA unit can operate at gas inlet temperatures of up to about 70, 65, 60, 55, 50, 45, 40, 35, 30, 25, 20, 15, 10, 5, 0, -5, -10, -15, -20, -25, -30, -45, -50 degrees Celsius or less. For example, the PSA can operate at a temperature above the temperature at which a component of the gas mixture condenses.
[0034] A cryogenic separation device may be configured to separate components (e.g., different gases of a gas mixture) using cryogenic (e.g., partially ambient) temperatures. For example, a cryogenic separation device may be configured to cool a mixture until all components of the mixture are condensed, and then remove the components (e.g., vaporize) to separate the components using an increase in temperature and / or pressure. Cryogenic separation may provide high purity of the components (e.g., hydrogen) of the gas mixture.
[0035] Once separated from the gas mixture, the hydrogen from the reactor can be further purified. In some cases, the hydrogen is of sufficient purity upon removal from the gas mixture (e.g., no further purification may be performed). In some cases, the hydrogen is purified by a PSA unit, a cryogenic separator, molecular sieves, or the like, or any combination thereof. In some cases, the hydrogen can be pressurized upon removal from the gas mixture. For example, the hydrogen can be pressurized before being fed to the purification unit. Following purification, the hydrogen can be of at least about 50, 60, 70, 80, 85, 90, 91, 92, 93, 94, 95, 96, 97, 98, 99, 99.9, 99.99, 99.999, 99.9999, 99.99999, 99.99999%, or more (e.g., mole percent, weight percent, or volume percent) purity. Following purification, the hydrogen may be up to about 99.99999, 99.9999, 99.999, 99.99, 99.9, 99, 98, 97, 96, 95, 94, 93, 92, 91, 90, 85, 80, 70, 60, 50% or less pure (e.g., mole percent, weight percent, or volume percent). Gases removed from the hydrogen during purification may include hydrocarbons (e.g., methane, ethane, ethylene, acetylene, propene, benzene, toluene, naphthalene, anthracene, etc.), hydrogen, nitrogen, hydrogen cyanide, carbon monoxide, noble gases (e.g., argon, neon, krypton, etc.), etc., or any combination thereof. The gas removed from the hydrogen may comprise at least about 1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 11, 12, 13, 14, 15, 16, 17, 18, 19, 20, 21, 22, 23, 24, 25 mole percent or more of the gas mixture. The gas removed from the hydrogen may comprise up to about 25, 24, 23, 22, 21, 20, 19, 18, 17, 16, 15, 14, 13, 12, 11, 10, 9, 8, 7, 6, 5, 4, 3, 2, 1 mole percent or less of the gas mixture.
[0036] FIG. 2 shows a schematic diagram of an example of an apparatus 200 according to the present disclosure, including a cross-sectional view of an example of the reactor 200. A feedstock may be fed to the reactor 201. At least one process gas (e.g., any non-feed gas fed to a reactor according to the present disclosure) may be fed (e.g., can be fed) to the reactor 200. Hot gas 202 may be generated (e.g., within the reactor) by using a heat generator (e.g., at the top of the reactor (not shown)). For example, hot gas 202 may be generated at the top of the reactor by using one or more AC electrodes (e.g., three or more AC electrodes), by using DC electrodes (e.g., concentric DC electrodes), or by using a resistance or induction heater. Hot gas may be generated by heating at least a subset of one or more gases (e.g., the feedstock alone or the feedstock combined with at least one process gas) using AC electrodes, DC electrodes, or resistance or induction heaters. Heating may include directly heating the hydrocarbons (e.g., the feedstock). For example, the hydrocarbon (e.g., feedstock) can be added to the heat generator (e.g., at a pressure as described elsewhere herein). For example, the hydrocarbon (e.g., feedstock) can be added by direct injection into the plasma. As described elsewhere herein, the reactor 201 can include a heat generator (not shown). In this configuration, the hydrocarbon (e.g., feedstock) can be heated in the same chamber as the carbonaceous material (also referred to herein as a "single chamber," "single stage reactor," or "single stage process") and / or hydrogen is produced (e.g., the formation of the plasma and the carbonaceous material / hydrogen can be in the same reactor). The reactor 201 can be configured to allow at least a portion or all of the flow in at least a portion of the reactor to be substantially axial, substantially radial, or a combination thereof. The reactor 201 (or at least a portion thereof, such as at least a portion of the inner wall of the reactor) can include a liner (e.g., a refractory liner). The hydrocarbon (e.g., feedstock) can be fed to the reactor.For example, the hydrocarbon (e.g., feedstock) may be injected into the reactor via one or more injectors (e.g., injectors 305, 406, 407, or any combination thereof). Alternatively or additionally, the hydrocarbon (e.g., feedstock) may be supplied via one or more inlet ports (e.g., in the wall of the reactor 200). Discussions herein regarding the number and / or location of injectors may equally apply to the inlet ports in at least some configurations, and vice versa. One or more process gases may be supplied via one or more inlet ports (e.g., the same or different as the hydrocarbon or feedstock) and / or via at least a subset of the one or more injectors. A given process gas may be supplied together with the feedstock, separately from the feedstock, or combinations thereof (e.g., a feedstock may be supplied to a given process gas, and either the given process gas or a different process gas may be supplied separately from the feedstock (e.g., as a purge)). A given process gas may or may not be heated by a heat generator. The feedstock may be supplied and / or a process gas may be supplied in parallel with the feedstock. The process gas may change the environment or atmosphere in / around at least a portion of the reactor, heat generator, inlet port and / or injector, purge at least a portion of the reactor, heat generator, inlet port and / or injector, or any combination thereof. For example, an inlet port, an array of inlet ports or a plenum (e.g., at the top of a reactor, such as reactors 201, 301 and / or 301) may be used to purge at least a portion of the reactor (e.g., one or more walls), one or more other inlet ports and / or one or more injectors (e.g., as described in more detail elsewhere herein). The description of an inlet port herein may equally apply to an array or plenum of inlet ports in at least some configurations, and vice versa. The one or more gases (e.g., feedstock alone or in combination with at least one process gas) heated with electrical energy may include substantially only hydrocarbons (e.g., feedstock).For example, the one or more gases heated with electrical energy may include the feedstock, may not include process gas, or may include some process gas with the addition of a purge level of process gas and / or feedstock (e.g., the one or more gases heated with electrical energy may include feedstock and process gas only at a purge level). Such a configuration may be referred to herein as a "once-through process" since the heated hydrocarbons (e.g., feedstock) include substantially only freshly fed hydrocarbons. Alternatively, the one or more gases heated with electrical energy may include a higher level of process gas. The level of a given process gas or the sum of a subset or all process gases (e.g., on a per mole feedstock basis) and the percentage of process gas heated with electrical energy may be as described elsewhere herein. In some cases, when DC electrodes are used, two electrodes may be used. In some cases, when DC electrodes are used, multiple two electrodes may be used (e.g., 2, 4, 6, etc.). AC electrodes may be used in a single-phase or three-phase configuration. If a single-phase AC configuration is used, multiple 2-electrodes may be used (e.g., 2, 4, 6, 8, etc.). If a three-phase AC configuration is used, multiple 3-electrodes can be used (e.g., 3, 6, 9, etc.). Each electrode can have an associated injector. For example, a three-phase three-electrode configuration can include three injectors positioned above the plane of the electrodes.
[0037] For example, hydrogen and carbonaceous materials (e.g., carbon particles) can be produced in a once-through, single-stage process that includes adding a hydrocarbon (e.g., natural gas) to a plasma generator at pressures above atmospheric pressure. The hydrocarbon may be added by direct injection (e.g., direct injection of the feedstock) into the plasma generated by the plasma generator. Energy from the plasma generator can remove the hydrogen from the hydrocarbon. The process can further include the use of heat exchangers, filters, and solids handling equipment. The solids handling equipment can include a cooled solid carbon collection screw conveyor, an airlock and purge system, a pneumatic conveying system, a classifying mill, and a product storage vessel.
[0038] The wear rate of the electrodes may be reduced or minimized as a result of the systems and methods described herein. The wear rate may be defined in units of wear in kg (mass of electrodes lost as a result of implementing the systems and methods described herein) per electrode per ton of carbon produced. In some cases, the wear rate of the one or more electrodes is between about 5 kg wear per electrode per ton of carbon produced and about 20 kg wear per electrode per ton of carbon produced. In some cases, the wear rate of the one or more electrodes is between about 5 kg wear per electrode per ton of carbon produced and about 10 kg wear per electrode per ton of carbon produced, between about 5 kg wear per electrode per ton of carbon produced and about 20 kg wear per electrode per ton of carbon produced, or between about 10 kg wear per electrode per ton of carbon produced and about 20 kg wear per electrode per ton of carbon produced. In some cases, the wear rate of the one or more electrodes is between about 5 kg wear per electrode per ton of carbon produced, between about 10 kg wear per electrode per ton of carbon produced, or between about 20 kg wear per electrode per ton of carbon produced. In some cases, the wear rate of the one or more electrodes is at least about 5 kg of wear per electrode per ton of carbon produced, or about 10 kg of wear per electrode per ton of carbon produced. In some cases, the wear rate of the one or more electrodes is up to about 10 kg of wear per electrode per ton of carbon produced, or about 20 kg of wear per electrode per ton of carbon produced.
[0039] FIG. 3 shows a schematic diagram of another example of an apparatus 300 according to the present disclosure, including a cross-sectional view of an example reactor 301 with a heat generator 302. The heat generator 302 can include AC electrodes 303 of a conductive material. The AC electrodes 303 can be arranged, for example, in a single-phase or three-phase configuration. One or more gases (e.g., feedstock alone or in combination with at least one process gas) 304 can flow between the electrodes, where an arc can excite it to a plasma state. At least a subset of the one or more gases (e.g., feedstock alone or in combination with at least one process gas) can be heated as described elsewhere herein (e.g., in connection with FIG. 2). The hydrocarbons (e.g., feedstock) can be injected through various injector configurations described herein (e.g., as described in connection with FIGS. 2 and 4). For example, the hydrocarbons (e.g., feedstock) can be injected into injector 305 (e.g., between the electrodes 302). The reactor can include an injector associated with each electrode. In FIG. 3, additional injectors may be omitted for clarity (e.g., the injectors may be blocked by the electrodes). The apparatus may include one or more electrode sliding seals 306. The electrode sliding seals may be configured to provide a gas seal of the apparatus (e.g., sealed so that gas does not leak from the apparatus under pressure). The electrode sliding seals may be configured to allow movement of the electrode within the apparatus while maintaining a gas seal of the apparatus. For example, an electrode can be fed into the apparatus as it wears, and the electrode sliding seal can maintain the atmosphere of the apparatus while the electrode is fed into the apparatus. A purge gas can be applied through the sliding seal 306 to maintain the environment of the reactor and prevent ingress of atmospheric gases through the seal. The purge gas can be as described elsewhere herein (e.g., process gas). The sliding seals may be configured to allow movement of the electrode within the reactor. For example, the seals can allow movement of the electrode into and / or out of the reactor. In another example, the seals can allow movement of the electrode within the three-dimensional space of the reactor. The hydrocarbon may be injected adjacent to one or more electrodes.The hydrocarbons can be injected in close proximity to one or more electrodes. In some cases, the hydrocarbons are injected at a distance of about 1 mm to about 1,000 mm from the electrodes. In some cases, the hydrocarbons are injected at a distance of about 1 mm to about 5 mm, about 1 mm to about 10 mm, about 1 mm to about 100 mm, about 1 mm to about 1,000 mm, about 5 mm to about 10 mm, about 5 mm to about 100 mm, about 5 mm to about 1,000 mm, about 10 mm to about 100 mm, about 10 mm to about 1,000 mm, or about 100 mm to about 1,000 mm. In some cases, the hydrocarbons are injected at a distance of about 1 mm, about 5 mm, about 10 mm, about 100 mm, or about 1,000 mm from the electrodes. In some cases, the hydrocarbons are injected at a distance of at least about 1 mm, about 5 mm, about 10 mm, or about 100 mm from the electrodes. In some cases, the hydrocarbon is injected at a distance from the electrode of up to about 5 mm, about 10 mm, about 100 mm, or about 1,000 mm.
[0040] The pressure at either tip of the injector may be the same as the ambient reactor pressure. In some cases, the pressure at either tip of the injector is greater than the ambient reactor pressure. In some cases, the pressure at either tip of the injector is within 20% of the ambient reactor pressure. In some cases, the pressure at either tip of the injector is within 10% of the ambient reactor pressure. In some cases, the pressure at either tip of the injector is within 5% of the ambient reactor pressure. In some cases, the pressure at either tip of the injector is within 1% of the ambient reactor pressure.
[0041] The electrode and / or injector can have a tilt angle (e.g., angle between the long axis of the electrode or injector and the long axis of the reactor) of at least about 0 degrees, 5 degrees, 10 degrees, 15 degrees, 20 degrees, 25 degrees, 30 degrees, 35 degrees, 40 degrees, 45 degrees, 50 degrees, 55 degrees, 60 degrees, 65 degrees, 70 degrees, 75 degrees, 80 degrees, 85 degrees, 90 degrees, or more. The electrode and / or injector may have a tilt angle of up to about 90, 85, 80, 75, 70, 65, 60, 55, 50, 45, 40, 35, 30, 25, 20, 15, 10, 5, 0 degrees, or less. The electrode and / or injector can have a tilt angle within a range defined by any two of the advance values. For example, the electrode and injector may have a tilt angle of about 15 to about 30 degrees. A higher tilt angle can increase the stability of the torch. The injector may include a heat resistant material (e.g., metal, tungsten, graphite, metal carbide, ceramic material, alumina, silica, aluminosilicate, glass, etc.). For example, the injector may be formed of a metal (e.g., copper, stainless steel, Inconel, etc.). The injector may be water cooled. The injector may be configured to deliver additional additives to the reactor in addition to the feedstock.
[0042] The reactor may include one or more optional sheath gas injectors. The sheath gas injectors may be configured to provide an inert gas configured to provide a barrier against coking within the reactor chamber. The inert gas may be as described elsewhere herein. The sheath gas may be located on the inner reactor side. The sheath gas may be elevated above the electrode tips. The sheath gas may be introduced into the reactor through slits on the periphery of the reactor configured to allow gas to flow from the slits in close proximity to the inner surface of the reactor.
[0043] The electrodes may be cylindrical in shape. The electrodes may be movable via a screw system that cooperates with a sliding seal associated with the electrodes. The screw system may be water-cooled. The use of a movable electrode allows for continuous operation of the reactor. For example, additional electrode material may be bonded to the end of the electrode outside the reactor, and new electrode material may be fed to the reactor as the electrode degrades within the reactor. In this example, the ability to add new electrode material outside the reactor while the reactor is operating can provide for continuous or substantially continuous operation of the reactor. In some cases, the electrodes include graphite (e.g., synthetic graphite, natural graphite, semi-graphite, etc.), a carbonaceous material and a resin or other binder, a carbon composite material, a carbon fiber material, etc., or any combination thereof. The electrodes may be at least about 1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 11, 12, 13, 14, 15, 16, 17, 18, 19, 20, 21, 22, 23, 24, 25, 26, 27, 28, 29, 30, 35, 40 inches or more in diameter. The electrodes may be up to about 40, 35, 30, 29, 28, 27, 26, 25, 24, 23, 22, 21, 20, 19, 18, 17, 16, 15, 14, 13, 12, 11, 10, 9, 8, 7, 6, 5, 4, 3, 2, 1 inch or less in diameter. The electrodes may be at least about 1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 11, 12, 13, 14, 15, 16, 17, 18, 19, 20, 21, 22, 23, 24 feet or more in length. The electrodes may be up to about 24, 23, 22, 21, 20, 19, 18, 17, 16, 15, 14, 13, 12, 11, 10, 9, 8, 7, 6, 5, 4, 3, 2, 1 feet or less in length. The distance between the center point of the electrode arc and the wall of the reactor may be at least about 0.1, 0.2, 0.3, 0.4, 0.5, 0.6, 0.7, 0.8, 0.9, 1, 1.1, 1.2, 1.3, 1.4, 1.5, 1.6, 1.7, 1.8, 1.9, 2, 2.1, 2.2, 2.3, 2.4, 2.5, 2.6, 2.7, 2.8, 2.9, 3, 3.1, 3.2, 3.3, 3.4, 3.5, 3.6, 3.7, 3.8, 3.9, 4 meters or more.The distance between the center point of the electrode arc and the wall of the reactor may be up to about 4, 3.9, 3.8, 3.7, 3.6, 3.5, 3.4, 3.3, 3.2, 3.1, 3, 2.9, 2.8, 2.7, 2.6, 2.5, 2.4, 2.3, 2.2, 2.1, 2, 1.9, 1.8, 1.7, 1.6, 1.5, 1.4, 1.3, 1.2, 1.1, 1, 0.9, 0.8, 0.7, 0.6, 0.5, 0.4, 0.3, 0.2, 1.2, or 0.1 meters or less. If the distance is too large, gas may recirculate back into the plasma region, and if the distance is too small, the wall of the reactor may deteriorate. In some cases, the electrodes can have a mass of at least about 20, 100, 200, 300, 400, 500, 600, 700, 800, 900, 1,000, 10,000, 20,000, 30,000, 40,000 kilograms or more. In some cases, the electrodes can have a mass of less than or equal to about 40,000, 30,000, 20,000, 10,000, 900, 800, 700, 600, 500, 400, 300, 200, 100, 20 kilograms.
[0044] FIG. 4 shows a schematic diagram of another example of an apparatus 400 according to the present disclosure, including a cross-sectional view of an example reactor 401 with a heat generator 402. The heat generator 402 can include inner and outer DC electrodes 403 and 404, respectively, comprising conductive material arranged concentrically (e.g., as concentric rings). One or more gases (e.g., feedstock alone or in combination with at least one process gas) 405 can flow between the electrodes 403 and 404, where an arc can excite it to a plasma state. The arc can be controlled by the use of a magnetic field that causes the arc to move rapidly in a circle around the electrode tip. The electrodes 403 and 404 may or may not be oriented parallel to the axis of the reactor 401 and / or each other. The electrodes 403 and / or 404 can include complex shapes. The hydrocarbons (e.g., feedstock) can be injected through various injector configurations described herein (e.g., as described in connection with FIG. 2 and FIG. 3). For example, the hydrocarbon (eg, feedstock) can be injected through injector 406 (eg, through the center of the concentric electrodes), through injector 407, or any combination thereof.
[0045] 2, 3 and 4, injector configurations according to the present disclosure may include a central injector (e.g., injector 406), one or more injectors (or arrays of injectors) located inside (e.g., replacing or in addition to the central injector) or between and / or outside (e.g., peripheral / surrounding) the electrodes of the heat generator (e.g., injector 305), or any combination thereof. The one or more injectors (or arrays of injectors) located inside, between and / or outside the electrodes of the heat generator may be oriented parallel to the axis of the reactor (e.g., injectors 406 and 407), or at an angle (e.g., inward) to the axis of the reactor (e.g., injector 305), and / or relative to each other. As described elsewhere herein, in some cases, a given injector flow may instead be fed through an inlet port. For example, a hydrocarbon (e.g., feedstock) may be provided as one or more gases 304 or injected via injector 406. The tips of the injectors may be located above the bottom surface of the electrode, below the plane, or in the same plane (e.g., flush with the plane). For example, in Figures 3 and 4, the tips of injectors 305, 406, and 407 are shown above the bottom surface of the electrode. One or more injectors of a given injector configuration may be cooled (e.g., a central injector, such as injector 406, may be cooled). An injector configuration may include, for example, 1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 11, 12, 13, 14, 15, 16, 17, 18, 19, 20, 21, 22, 23, 24, or 25 or more injectors. Alternatively or additionally, the injector configuration may comprise less than or equal to 50, 40, 30, 25, 24, 23, 22, 21, 20, 19, 18, 17, 16, 15, 14, 13, 12, 11, 10, 9, 8, 7, 6, 5, 4, or 3 injectors, for example. For example, the injector configuration can include a central injector and an array of injectors around the central injector (disposed inward, between, and / or outward of the electrodes), an array of injectors without a central injector (disposed inward, between, and / or outward of the electrodes), etc.The injectors can be configured to feed the hydrocarbons in multiple injection streams (e.g., at least about 2, 3, 4, 5, 6, 7, 8, 9, 10 or more injection streams). The multiple injection streams can be above the plane of the electrodes in the reactor, and a second set of injectors can be configured to inject below the plane of the electrodes. For example, a first set of injectors can feed the hydrocarbon feed above the electrodes in the reactor, and a second set of injectors can feed the hydrocarbon feed in a plane below the electrodes in the reactor. The plane of the electrodes can be a plane perpendicular to the length of the reactor such that the tip of each electrode is within at least about 0.01, 0.05, 0.1, 0.2, 0.3, 0.4, 0.5 meters or more of the plane. The plane of the electrodes can be a plane perpendicular to the length of the reactor such that the tip of each electrode is within at most about 0.5, 0.4, 0.3, 0.2, 0.1, 0.05, 0.01 meters or less of the plane. In some cases, a Joule heating (e.g., resistive heating) source can be used in place of a plasma heating source as described elsewhere herein. For example, a resistive heating element can be placed in the reactor in place of a plasma torch and configured to provide the heat used for the reaction.
[0046] An injector (or a portion thereof) according to the present disclosure (e.g., injector 305, 406, 407, or any combination thereof) may include or be one or more suitable materials, such as, for example, copper, stainless steel, graphite, alloys (e.g., high temperature corrosion resistant metals), and / or other similar materials (e.g., having high melting points and good corrosion resistance). The injector may be cooled via a cooling fluid. The injector may be cooled, for example, by water or a non-oxidizing liquid (e.g., mineral oil, ethylene glycol, propylene glycol, synthetic organic fluids such as DOWTHERM™ materials, etc.).
[0047] The heat generator (e.g., plasma generator) and / or reactor (or portions thereof) of the present disclosure may include or be made of, for example, copper, tungsten, graphite (e.g., extruded or molded), molybdenum, rhenium, nickel, chromium, iron, silver, other refractory or high temperature metals, or alloys thereof (e.g., copper-tungsten alloy, rhenium-tungsten alloy, molybdenum-tungsten alloy, or copper-rhenium alloy; carbide alloys such as tungsten carbide, molybdenum carbide, or chromium carbide; etc.), boron nitride, silicon carbide, alumina, alumina-silica blends, or other high temperature ceramics; other oxidation-resistant refractory materials; or any combination thereof. At least a portion of the electrodes (e.g., one or both of electrodes 303, 403, and 404) of the heat generator (e.g., plasma generator) may include one or more of the aforementioned materials. The electrodes according to the present disclosure can have any suitable shape (e.g., bars with cylindrical, elliptical or polygonal cross-sections, pointed or rounded ends, etc.). The electrode shape may be customized. Alternatively, the heat generator may be configured to allow for integration of existing electrode shapes (e.g., used in steelmaking). The electrode material (e.g., chemical composition, grain structure, etc.) and / or shape may be configured to enhance survivability (e.g., strength, thermal flexibility, etc.). At least a portion of the reactor (e.g., at least a portion of the wall or liner) according to the present disclosure may include one or more of the aforementioned materials (e.g., the reactor may be lined with refractory). The reactor (e.g., the wall or liner of the reactor) may include one or more sections including different materials. For example, a refractory liner may include one or more sections including different refractories, e.g., a section that may be too high for a given refractory, and another section including a given (e.g., standard) refractory.
[0048] A thermal generator (e.g., a plasma generator) according to the present disclosure can be configured such that, for example, about 750 kilograms (kg), 500 kg, 400 kg, 300 kg, 200 kg, 100 kg, 90 kg, 80 kg, 70 kg, 60 kg, 50 kg, 40 kg, 30 kg, 20 kg, 15 kg, 10 kg, 5 kg, 2 kg, 1.75 kg, 1.5 kg, 1.25 kg, 1 kg, 0.9 kg, 0.8 kg, 0.7 kg, 0.6 kg, 500 g (g), 400 g, 300 g, 200 g, 100 g, 50 g, 20 g, 10 g, 5 g, 2 g, or 1 g or less of electrode material (e.g., electrode 303, and / or electrodes 403 and 404) is consumed per ton (e.g., metric ton) of carbonaceous material (e.g., solid carbonaceous material) produced. Alternatively or additionally, a thermal generator (e.g., plasma generator) of the present disclosure may be configured such that, for example, about 0 g, 1 g, 1.25 kg, 1.5 kg, 1.75 kg, 2 g, 5 g, 10 g, 20 g, 50 g, 100 g, 200 g, 300 g, 400 g, 500 g, 0.6 kg, 0.7 kg, 0.8 kg, 0.9 kg, 1 kg, 2 kg, 5 kg, 10 kg, 15 kg, 20 kg, 30 kg, 40 kg, 50 kg, 60 kg, 70 kg, 80 kg, 90 kg, 100 kg, 200 kg, 300 kg, 400 kg, or 500 kg or more of electrode material (e.g., electrode 303, and / or electrodes 403 and 404) is consumed per ton (e.g., metric ton) of carbonaceous material (e.g., solid carbonaceous material) produced.
[0049] Electrodes (e.g., AC and / or DC electrodes of a plasma generator) (or portions thereof) (e.g., electrode 303, and / or electrodes 403 and 404) according to the present disclosure can be positioned at a given distance (also referred to herein as a "gap" or "gap size") from one another. The gap between the electrodes (or portions thereof) can be, for example, about 40 millimeters (mm), 39 mm, 38 mm, 37 mm, 36 mm, 35 mm, 34 mm, 33 mm, 32 mm, 31 mm, 30 mm, 29 mm, 28 mm, 27 mm, 26 mm, 25 mm, 24 mm, 23 mm, 22 mm, 21 mm, 20 mm, 19 mm, 18 mm, 17 mm, 16 mm, 15 mm, 14 mm, 13 mm, 12 mm, 11 mm, 10 mm, 9 mm, 8 mm, 7 mm, 6 mm, 5 mm, 4 mm, 3 mm, 2 mm, or 1 mm or less. Alternatively or additionally, the gap between the electrodes (or portions thereof) may be, for example, about 0.5 mm, 1 mm, 2 mm, 3 mm, 4 mm, 5 mm, 6 mm, 7 mm, 8 mm, 9 mm, 10 mm, 11 mm, 12 mm, 13 mm, 14 mm, 15 mm, 16 mm, 17 mm, 18 mm, 19 mm, 20 mm, 21 mm, 22 mm, 23 mm, 24 mm, 25 mm, 26 mm, 27 mm, 28 mm, 29 mm, 30 mm, 31 mm, 32 mm, 33 mm, 34 mm, or 35 mm or more.
[0050] The hydrocarbon feedstock is a compound of formula C n H x Or C n H x O ywhere n is an integer, x is (i) between 1 and 2n+2, or (ii) less than 1 for fuels such as coal, coal tar, pyrolysis fuel oil, and y is between 0 and n. Hydrocarbon feedstocks may include, for example, simple hydrocarbons (e.g., methane, ethane, propane, butane, etc.), aromatic feedstocks (e.g., benzene, toluene, xylene, methylnaphthalene, pyrolysis fuel oil, coal tar, coal, heavy fuel oil, oil, bio-oil, biodiesel, other biologically derived hydrocarbons, etc.), unsaturated hydrocarbons (e.g., ethylene, acetylene, butadiene, styrene, etc.), oxygenated hydrocarbons (e.g., ethanol, methanol, propanol, phenol, ketones, ethers, esters, etc.), or any combination thereof. These examples are provided as non-limiting examples of acceptable hydrocarbon feedstocks that can be further combined and / or mixed with other components for production. Hydrocarbon feedstocks may refer to feedstocks where a majority of the feedstock (e.g., greater than about 50% (by weight)) is hydrocarbon in nature. The reactive hydrocarbon feedstock may include at least about 70% (by weight) methane, ethane, propane, or mixtures thereof. The hydrocarbon feedstock may include or be natural gas. The hydrocarbons may include or be methane, ethane, propane, or mixtures thereof. The hydrocarbons may include methane, ethane, propane, butane, acetylene, ethylene, carbon black oil, coal tar, crude coal tar, diesel oil, benzene, and / or methylnaphthalene. The hydrocarbons may include (e.g., additional) polycyclic aromatic hydrocarbons. The hydrocarbon feedstock may include one or more simple hydrocarbons, one or more aromatic feedstocks, one or more unsaturated hydrocarbons, one or more oxygenated hydrocarbons, or any combination thereof.The hydrocarbon feedstock may include, for example, methane, ethane, propane, butane, pentane, natural gas, benzene, toluene, xylene, ethylbenzene, naphthalene, methylnaphthalene, dimethylnaphthalene, anthracene, methylanthracene, other monocyclic or polycyclic aromatic hydrocarbons, carbon black oil, diesel oil, pyrolysis fuel oil, coal tar, crude coal tar, coal, heavy oil, oil, bio-oil, biodiesel, other biologically derived hydrocarbons, ethylene, acetylene, propylene, butadiene, styrene, ethanol, methanol, propanol, phenol, one or more ketones, one or more ethers, one or more esters, one or more aldehydes, or any combination thereof. The feedstock may also include one or more derivatives of the feedstock compounds described herein (e.g., among the aforementioned feedstocks), such as benzene and / or derivatives thereof, naphthalene and / or derivatives thereof, anthracene and / or derivatives thereof, etc. The hydrocarbon feedstock (also referred to herein as "feedstock") may contain less than about 1 ppm, 5 ppm, 10 ppm, 25 ppm, 50 ppm, 0.01%, 0.05%, 0.1%, 0.2%, 0.3%, 0.4%, 0.5%, 0.6%, 0.7%, 0.8%, 0.9%, 1%, 1.1%, 1.2%, 1.3%, 1.4%, 1.5%, 1.6%, 1.7%, 1.8%, 1.9%, 2%, 2.5%, 3%, 3.5%, 4%, 4.5%, 5%, 6%, 7%, 8%, 9%, 10%, 11%, 12%, 13%, 14%, 15%, 16%, 17%, 18%, 19%, 20%, 21%, 22%, 23%, 24%, 25%, 26%, 27%, 28%, 29%, 30%, 31%, 32%, 33%, 34%, 35%, 36%, 37%, 38%, 39%, 40%, 41%, 42%, 43%, 44%, 45%, 46%, 47%, 48%, 49%, 50%, 51%, 52%, 53%, 54%, 55%, 56%, 57%, 58%, 59%, 60%, 61%, 62%, 63%, 64%, 65%, 66%, 67%, 68%, 69%, 70%, 71%, 72%, 73%, 74%, 75%, 76%, 77%, 78%, 79%, 80%, 81%, 82%, 83%, 84%, 85%, 86%, 87%, 88%, 89%, 90 %, 16%, 17%, 18%, 19%, 20%, 21%, 22%, 23%, 24%, 25%, 26%, 27%, 28%, 29%, 30%, 31%, 32%, 33%, 34%, 35%, 36%, 37%, 38%, 39%, 40%, 41%, 42%, 43%, 44%, 45%, 46%, 47%, 48%, 49%, 50%, 55%, 60%, 65%, 70%, 75%, 80%, 85%, 90%, 95% or 99% or more of a given feedstock (among the aforementioned feedstocks) (e.g., in a mixture of feedstocks).Alternatively or in addition, the feedstock may be at least about 100%, 99%, 95%, 90%, 85%, 80%, 75%, 70%, 65%, 60%, 55%, 50%, 49%, 48%, 47%, 46%, 45%, 44%, 43%, 42%, 41%, 40%, 39%, 38%, 37%, 36%, 35%, 34%, 33%, 32%, 31%, 30%, 29%, 28%, 27%, 26%, 25%, 24%, 23%, 22%, 21%, 20%, 19%, 18%, 17%, 16%, 15%, 14%, 18%, 19%, 20%, 21%, 22%, 23%, 24%, 25%, 25%, 26%, 27%, 27%, 28%, 29%, 29%, 30 ... The given feedstock may include a concentration (e.g., in the feedstock mixture) of 3%, 12%, 11%, 10%, 9%, 8%, 7%, 6%, 5%, 4, 5%, 4%, 3.5%, 3%, 2.5%, 2%, 1.9%, 1.8%, 1.7%, 1.6%, 1.5%, 1.4%, 1.3%, 1.2%, 1.1%, 1%, 0.9%, 0.8%, 0.7%, 0.6%, 0.5%, 0.4%, 0.3%, 0.2%, 0.1%, 0.05%, 0.01%, 50 ppm, 25 ppm, 10 ppm, 5 ppm, or 1 ppm or less of the given feedstock. The feedstock may include additional feedstocks (e.g., in the feedstock mixture) of similar or different concentrations. Such additional feedstocks may be selected, for example, from among the aforementioned feedstocks not selected as the given feedstock. The given feedstock may itself include a mixture (e.g., natural gas, etc.).
[0051] The process gas can include, for example, oxygen, nitrogen, argon, helium, air, hydrogen, carbon monoxide, water, hydrocarbons (e.g., methane, ethane, unsaturated and / or any of the hydrocarbons described herein in connection with the feedstock), etc. (used alone or in mixtures of two or more). In some examples, the process gas may be inert. The process gas may include or be freshly supplied gas (e.g., delivered or supplied from a reservoir such as a cylinder or vessel), recycled gaseous reaction products (e.g., as described in more detail elsewhere herein), or any combination thereof. The process gas may be, for example, oxygen, nitrogen (e.g., up to about 30% by volume), argon (e.g., up to about 30% Ar), helium, air, hydrogen (e.g., about 50%, 60%, 70%, 80%, and 90% or more, up to about 100% by volume), carbon monoxide (e.g., at least about 1 ppm by volume up to about 30%), water, hydrocarbons (e.g., methane, ethane, unsaturated, benzene and toluene or similar monoaromatic hydrocarbons, polycyclic aromatic hydrocarbons such as anthracene and its derivatives, naphthalene and its derivatives, methylnaphthalene, methylanthracene, coronene, pyrene ... The process gas may include (used alone or in mixtures of two or more) at least about 60% to about 100% hydrogen (by volume) and may further include up to about 30% nitrogen, up to about 30% CO, up to about 30% CH, up to about 10% H, up to about 10% H by volume, and / or at least about 1 ppm polyaromatic hydrocarbons by volume. The process gas may include at least about 60% to about 100% hydrogen (by volume) and may further include up to about 30% nitrogen, up to about 30% CO, up to about 30% CH, up to about 10% HCN, up to about 30% CH, and up to about 30% Ar. For example, the process gas may be greater than about 60% hydrogen. Additionally, the process gas may also include polycyclic aromatic hydrocarbons, such as anthracene, naphthalene, coronene, pyrene, chrysene, fluorene, and the like.Additionally, the process gas may have benzene and toluene or similar monoaromatic hydrocarbon components present. For example, the process gas may include about 90% or more hydrogen, and about 0.2% nitrogen, about 1.0% CO, about 1.1% CH4, about 0.1% HCN, and about 0.1% C2H2. The process gas may include about 80% or more hydrogen, with the remainder including some mixture of the aforementioned gases, polycyclic aromatic hydrocarbons, monoaromatic hydrocarbons, and other components. The process gas may include about 50% or more hydrogen by volume. The process gas may include more than about 70% H2 by volume, and may include at least one or more of the gases HCN, CH4, C2H4, C2H2, CO, benzene, or polyaromatic hydrocarbons (e.g., naphthalene and / or anthracene) at a level of at least about 1 ppm. The polyaromatic hydrocarbons may include, for example, naphthalene, anthracene, and / or their derivatives. The polyaromatic hydrocarbons may include, for example, methylnaphthalene and / or methylanthracene.The process gas may be selected from the group consisting of a process gas concentration of about 1 ppm, 5 ppm, 10 ppm, 25 ppm, 50 ppm, 0.01%, 0.05%, 0.1%, 0.2%, 0.3%, 0.4%, 0.5%, 0.6%, 0.7%, 0.8%, 0.9%, 1%, 1.1%, 1.2%, 1.3%, 1.4%, 1.5%, 1.6%, 1.7%, 1.8%, 1.9%, 2%, 2.5%, 3%, 3.5%, 4%, 4.5%, 5%, 6%, 7%, 8%, 9%, 10%, 11%, 12%, 13%, 14%, 15%, 16%, 17%, 18%, 19%, 20%, 21%, 22%, 23%, 24%, 25%, 26%, 27%, 28%, 29%, 30%, 31%, 32%, 33%, 34%, 35%, 36%, 37%, 38%, 39%, 40%, 41%, 42%, 43%, 44%, 45%, 46%, 47%, 48%, 49%, 50%, 51%, 52%, 53%, 54%, 55%, 56%, 57%, 58%, 59%, 60%, 61%, 62%, 63%, 64%, 65%, 66%, 67%, 68%, 69%, 70%, 71%, 72%, 73%, 74%, 75%, 76%, 77%, 78%, 79%, 80%, 81%, 82%, 83%, 84%, 85%, 86%, 87%, 88%, 89%, 90%, 91 %,12%,13%,14%,15%,16%,17%,18%,19%,20%,21%,22%,23%,24%,25%,26%,27%,28%,29%,30%,31%,32%,33%,34%,35%,36%,37%,38%,39%,40%,41%,42%,43%,44%,45%,46%,47%,48%,49%,50%,55%,60%,65%,70%,75%,80%,85%,90%,95% or 99% or more (e.g., in a process gas mixture). Alternatively or additionally, the process gas may be about 100%, 99%, 95%, 90%, 85%, 80%, 75%, 70%, 65%, 60%, 55%, 50%, 49%, 48%, 47%, 46%, 45%, 44%, 43%, 42%, 41%, 40%, 39%, 38%, 37%, 36%, 35%, 34%, 33%, 32%, 31%, 30%, 29%, 28%, 27%, 26%, 25%, 24%, 23%, 22%, 21%, 20%, 19%, 18%, 17%, 16% by weight, volume or moles of a given process gas. , 15%, 14%, 13%, 12%, 11%, 10%, 9%, 8%, 7%, 6%, 5%, 4, 5%, 4%, 3.5%, 3%, 2.5%, 2%, 1.9%, 1.8%, 1.7%, 1.6%, 1.5%, 1.4%, 1.3%, 1.2%, 1.1%, 1%, 0.9%, 0.8%, 0.7%, 0.6%, 0.5%, 0.4%, 0.3%, 0.2%, 0.1%, 0.05%, 0.01%, 50 ppm, 25 ppm, 10 ppm, 5 ppm or 1 ppm or less (e.g., in a process gas mixture). The process gas may include additional process gases (e.g., in a process gas mixture) of similar or different concentrations.Such additional process gases may be selected, for example, from among the aforementioned process gases not selected as the given process gas. The given process gas may itself comprise a mixture. The process gas may be used as a purge gas. The purge gas may be an inert gas used to purge the reactor or carbon particles (e.g., to remove non-inert gases). The purge gas may be provided at a pressure higher than the operating pressure of the reactor (e.g., the purge gas may be provided at a higher pressure in the reactor and adjusted to a lower pressure).
[0052] The feedstock (e.g., hydrocarbon) may be, for example, at about 50 grams / hour (g / hr), 100 g / hr, 250 g / hr, 500 g / hr, 750 g / hr, 1 kilogram / hour (kg / hr), 2 kg / hr, 5 kg / hr, 10 kg / hr, 15 kg / hr, 20 kg / hr, 25 kg / hr, 30 kg / hr, 35 kg / hr, 40 kg / hr, 45 kg / hr, 50 kg / hr, 55 kg / hr ,60kg / hr,65kg / hr,70kg / hr,75kg / hr,80kg / hr,85kg / hr,90kg / hr,95kg / hr,100kg / hr,150kg / hr,200kg / hr,250kg / hr,300kg / hr,350kg / hr,400kg / hr,450kg / hr,500kg / hr,600kg / hr,700kg / hr,800kg / hr,900 kg / hr,1,000kg / hr,1,100kg / hr,1,200kg / hr,1,300kg / hr,1,400kg / hr,1,500kg / hr,1,600kg / hr,1,700 kg / hr,1,800kg / hr,1,900kg / hr,2,000kg / hr,2,100kg / hr,2,200kg / hr,2,300kg / hr,2,400kg / hr,2,500 The feed may be supplied to the system (e.g., to a reactor such as reactor 102, 201, 301 or 401 described herein) at a rate of 1,000 kg / hr, 2,000 kg / hr, 3,500 kg / hr, 4,000 kg / hr, 4,500 kg / hr, 5,000 kg / hr, 6,000 kg / hr, 7,000 kg / hr, 8,000 kg / hr, 9,000 kg / hr or 10,000 kg / hr or more.Alternatively or additionally, the feedstock (e.g., hydrocarbon) may be, for example, about 10,000 kg / hr, 9,000 kg / hr, 8,000 kg / hr, 7,000 kg / hr, 6,000 kg / hr, 5,000 kg / hr, 4,500 kg / hr, 4,000 kg / hr, 3,500 kg / hr, 3,000 kg / hr, 2,500 kg / hr, 2,400 kg / hr ,2,300kg / hr,2,200kg / hr,2,100kg / hr,2,000kg / hr,1,900kg / hr,1,800kg / hr,1,700kg / hr,1,600 kg / hr,1,500kg / hr,1,400kg / hr,1,300kg / hr,1,200kg / hr,1,100kg / hr,1,000kg / hr,900kg / hr,80 0kg / hr,700kg / hr,600kg / hr,500kg / hr,450kg / hr,400kg / hr,350kg / hr,300kg / hr,250kg / hr,200k g / hr,150kg / hr,100kg / hr,95kg / hr,90kg / hr,85kg / hr,80kg / hr,75kg / hr,70kg / hr,65kg / hr,60kg / hr, 55 kg / hr, 50 kg / hr, 45 kg / hr, 40 kg / hr, 35 kg / hr, 30 kg / hr, 25 kg / hr, 20 kg / hr, 15 kg / hr, 10 kg / hr, 5 kg / hr, 2 kg / hr, 1 kg / hr, 750 g / hr, 500 g / hr, 250 g / hr or 100 g / hr.
[0053] Dilution can be the ratio of the total moles of process gas (e.g., diluent gas) to the total moles of carbon atoms (e.g., feed carbon atoms) injected into the reactor (e.g., during the processes described elsewhere herein). A dilution factor of less than about 2 can be beneficial in the operation of a plasma-based pyrolysis reactor. Achieving a dilution factor of less than about 2 can include using a hydrocarbon as the plasma gas. For example, a hydrocarbon can be used as both the plasma gas and the feed gas. A reactor having a dilution factor of less than about 2 can have recycle gas and purge gas in the immediate vicinity of the electrodes in an amount that provides a dilution factor of less than about 2. The purge gas may be present to pressurize the reactor and / or to pressurize sliding seals on the electrodes of the reactor. The devices and methods of the present disclosure can achieve dilution factors of at least about 0, 0.1, 0.2, 0.3, 0.4, 0.5, 0.6, 0.7, 0.8, 0.9, 1, 1.1, 1.2, 1.3, 1.4, 1.5, 1.6, 1.7, 1.8, 1.9, 2, 2.1, 2.2, 2.3, 2.4, 2.5, 2.6, 2.7, 2.8, 2.9, 3, 3.1, 3.2, 3.3, 3.4, 3.5, 3.6, 3.7, 3.8, 3.9, 4, or more. The disclosed apparatus and methods can achieve dilution factors of up to about 4, 3.9, 3.8, 3.7, 3.6, 3.5, 3.4, 3.3, 3.2, 3.1, 3, 2.9, 2.8, 2.7, 2.6, 2.5, 2.4, 2.3, 2.2, 2.1, 2, 1.9, 1.8, 1.7, 1.6, 1.5, 1.4, 1.3, 1.2, 1.1, 1, 0.9, 0.8, 0.7, 0.6, 0.5, 0.4, 0.3, 0.2, 0.1, or less.
[0054] Recycle gas can be provided to the reactor and method of the present disclosure. The recycle gas can be at least a component of the plasma gas. For example, the recycle gas can be provided to the reactor to be heated as part of the plasma gas. The recycle gas can be a process gas as described elsewhere herein. The recycle gas can be at least a portion of the gas produced by the reactor. For example, the recycle gas can be gas output by the reactor during the production of carbon particles and / or hydrogen. The recycle gas can include hydrogen (e.g., at least about 10, 20, 30, 40, 50, 60, 70, 80, 90, 99 percent or more hydrogen), nitrogen, argon, carbon monoxide, water, hydrocarbons, etc., or any combination thereof. The recycle gas can be gas rejected from a purification process as described elsewhere herein. For example, impurities removed from the hydrogen produced in a high pressure degasser can be used as the recycle gas. The recycle gas can be at an elevated temperature (e.g., above ambient). For example, the recycle gas can be provided at an elevated temperature to reduce the amount of energy lost from the plasma in heating the recycle gas. The use of recycle gas can increase efficiency by recycling reactants (e.g., hydrocarbons) back to the reactor, as well as extending the life of the electrodes in the reactor. For example, the hydrocarbons can be recycled back to the reactor, thereby improving the conversion of the hydrocarbons. The recycle gas can be introduced into the reactor via a sheath and / or blanket flow of the recycle gas and / or another inert gas, as described elsewhere herein. Such a flow can prevent deposition of gaseous and / or solid carbon on the electrodes and / or other surfaces of the reactor (e.g., reactor walls). In some cases, the recycle gas can be pressurized before being introduced into the reactor (e.g., recuring). For example, the recycle gas can be passed through a compressor before being injected into the reactor. The recycle gas can be pressurized to a pressure, as described elsewhere herein.
[0055] A given process gas or a subset or all of the process gases may have a flow rate of, for example, about 0 standard cubic meters per hour (Nm 3 / hr), 0.1Nm 3 / hr,0.2Nm 3 / hr,0.5Nm 3 / hr,1Nm 3 / hr, 1.5Nm 3 / hr,2Nm 3 / hr,5Nm 3 / hr,10Nm 3 / hr,25Nm 3 / hr,50Nm 3 / hr,75Nm 3 / hr,100Nm 3 / hr, 150Nm 3 / hr,200Nm 3 / hr,250Nm 3 / hr,300Nm 3 / hr, 350Nm 3 / hr, 400Nm 3 / hr, 450Nm 3 / hr,500Nm 3 / hr,550Nm 3 / hr,600Nm 3 / hr, 650Nm 3 / hr,700Nm 3 / hr,750Nm 3 / hr,800Nm 3 / hr,850Nm 3 / hr,900Nm 3 / hr,950Nm 3 / hr, 1,000Nm 3 / hr, 2,000Nm 3 / hr, 3,000Nm 3 / hr, 4,000Nm 3 / hr, 5,000Nm 3 / hr, 6,000Nm 3 / hr, 7,000Nm 3 / hr, 8,000Nm 3 / hr, 9,000Nm 3 / hr, 10,000Nm 3 / hr, 12,000Nm 3 / hr, 14,000Nm 3 / hr, 16,000Nm3 / hr, 18,000Nm 3 / hr, 20,000Nm 3 / hr, 30,000Nm 3 / hr, 40,000Nm 3 / hr, 50,000Nm 3 / hr, 60,000Nm 3 / hr, 70,000Nm 3 / hr, 80,000Nm 3 / hr, 90,000Nm 3 / hr or 15,000Nm 3 / hr or more. Alternatively or additionally, a given process gas or a subset or the sum of all process gases may be fed to the system (e.g., a reactor such as reactor 102, 201, 301 or 401 described herein) at a rate of, for example, about 100,000 Nm 3 / hr, 90,000Nm 3 / hr, 80,000Nm 3 / hr, 70,000Nm 3 / hr, 60,000Nm 3 / hr, 50,000Nm 3 / hr, 40,000Nm 3 / hr, 30,000Nm 3 / hr, 20,000Nm 3 / hr, 18,000Nm 3 / hr, 16,000Nm 3 / hr, 14,000Nm 3 / hr, 12,000Nm 3 / hr, 10,000Nm 3 / hr, 9,000Nm 3 / hr, 8,000Nm 3 / hr, 7,000Nm 3 / hr, 6,000Nm 3 / hr, 5,000Nm 3 / hr, 4,000Nm 3 / hr, 3,000Nm 3 / hr, 2,000Nm 3 / hr, 1,000Nm 3 / hr,950Nm 3 / hr,900Nm 3 / hr,850Nm3 / hr, 800 Nm 3 / hr, 750 Nm 3 / hr, 700 Nm 3 / hr, 650 Nm 3 / hr, 600 Nm 3 / hr, 550 Nm 3 / hr, 500 Nm 3 / hr, 450 Nm 3 / hr, 400 Nm 3 / hr, 350 Nm 3 / hr, 300 Nm 3 / hr, 250 Nm 3 / hr, 200 Nm 3 / hr, 150 Nm 3 / hr, 100 Nm 3 / hr, 75 Nm 3 / hr, 50 Nm 3 / hr, 25 Nm 3 / hr, 10 Nm 3 / hr, 5 Nm 3 / hr, 2 Nm 3 / hr, 1.5 Nm 3 / hr, 1 Nm 3 / hr, 0.5 Nm 3 / hr or 0.2 Nm 3 / hr or less. A given process gas or a subset or the sum of all process gases may be provided to a system (e.g., a reactor) at such rates in combination with one or more feed flow rates described herein. A given process gas or a subset or the sum of all process gases may be provided to a system (e.g., a reactor) at such rates in combination with one or more feed flow rates described herein. A given process gas or a subset or the sum of all process gases may be provided to a system (e.g., provided to a heat generator, e.g., heat generator 302 or 402, and / or provided elsewhere or entirely to a reactor, e.g., reactor 102, 201, 301 or 401 described herein) at a ratio of, for example, about 0, 0.0005, 0.001, 0.002, 0.005, 0.1, 0.2, 0.5, 1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 15, 20, 25, 30, 35, 40, 45, 50, 75, or 90 moles of process gas or more per mole of feedstock. Alternatively or additionally, a given process gas or a subset or the sum of all process gases may be supplied to the system (e.g., provided to a heat generator, such as, for example, heat generator 302 or 402, and / or provided elsewhere or entirely to a reactor, such as, for example, reactor 102, 201, 301 or 401 described herein) at a ratio of, for example, about 100, 90, 75, 50, 45, 40, 35, 30, 25, 20, 15, 10, 9, 8, 7, 6, 5, 4, 3, 2, 1, 0.5, 0.2, 0.1, 0.005, 0.002, 0.001, or 0.0005 moles of process gas or less per mole of feedstock. About 100%, 75%, 50%, 40%, 30%, 20%, 10%, 5%, or 1% or less of the process gas supplied to the system may be heated with electrical energy. Alternatively or additionally, about 0%, 1%, 5%, 10%, 20%, 30%, 40%, 50%, or 75% or more of the process gas supplied to the system may be heated with electrical energy.
[0056] One or more gases (e.g., a feedstock, alone or in combination with at least one process gas) can be heated at a given pressure. The feedstock (e.g., alone or in combination with at least one process gas) can be reacted at a given pressure (also referred to herein as the "reaction pressure"). The heating and reaction can be carried out in a reactor at a given pressure (also referred to herein as the "reactor pressure"). The pressure is, for example, about 0bar, 0.5bar, 1bar, 1.1bar, 1.2bar, 1.3bar, 1.4bar, 1.5bar, 1.6bar, 1.7bar, 1.8bar, 1.9bar, 2bar, 2.1bar, 2.2bar, 2.3bar. ,2.4bar,2.5bar,2.6bar,2.7bar,2.8bar,2.9bar,3bar,3.1bar,3.2bar,3.3bar,3.4bar,3.5bar,3.6bar,3.7bar,3.8bar,3.9bar,4ba r, 4.5 bar, 5 bar, 6 bar, 7 bar, 8 bar, 9 bar, 10 bar, 11 bar, 12 bar, 13 bar, 14 bar, 15 bar, 16 bar, 17 bar, 18 bar, 19 bar, 20 bar, 21 bar, 22 bar, 23 bar, 24 bar, 25 bar, 26 bar, 27 bar, 28 bar, 29 bar, 30 bar, 35 bar, 40 bar, 45 bar, 50 bar, 55 bar, 60 bar, 65 bar, 70 bar, 75 bar, or more.Alternatively or additionally, the pressure may be, for example, about 100 bar, 90 bar, 80 bar, 75 bar, 70 bar, 65 bar, 60 bar, 55 bar, 50 bar, 45 bar, 40 bar, 35 bar, 30 bar, 29 bar, 28 bar, 27 bar, 26 bar, 25 bar, 24 bar, 23 bar, 22 bar, 21 bar, 20 bar, 19 bar, 18 bar, 17 bar, 16 bar, 15 bar, 14 bar, 13 bar, 12 bar, 11 bar, 10 bar, 9 bar, 8 bar, 7 The pressure may be greater than atmospheric pressure (higher than atmospheric pressure). The pressure may be from about 1.5 bar to about 25 bar. The pressure may be from about 1 bar to about 70 bar. The pressure may be from about 5 bar to about 25 bar. The pressure may be from about 10 bar to about 20 bar. The pressure may be from about 5 bar to about 15 bar. The pressure may be about 2 bar or more. The pressure may be about 5 bar or more. The pressure may be about 10 bar or more. The feedstock and / or process gas may be supplied to the reactor at an appropriate pressure (e.g., at least about 0.01%, 0.05%, 0.1%, 0.5%, 1%, 2%, 5%, 10%, 15%, 20%, 25%, or 50% higher than the reactor pressure, which may depend on the mode of injection, e.g., higher pressure through the injector than through the inlet port). The feedstock and / or process gas may be supplied to the reactor, for example, at their respective delivery or storage (e.g., cylinder or vessel) pressure. The feedstock and / or process may or may not be compressed (e.g., further) before being supplied to the reactor. The inlet feedstock may be supplied at a pressure in a range defined by any two of the proceeding pressure values.For example, the feedstock can be provided at a pressure of about 30 to about 35 bar and can be metered to a pressure of about 5 to about 15 bar. There can be a pressure drop across the reactor. For example, the reactor inlet pressure and the reactor outlet pressure can be different. The reactor outlet pressure can be a value selected from the progression list that is less than the inlet pressure selected from the progression list. For example, a reactor having an inlet pressure of about 15 bar can have an outlet pressure of about 14 bar. In another example, the inlet pressure can be about 4 bar and the outlet pressure can be about 2 bar. In another example, the inlet pressure can be about 35 bar and the outlet pressure can be about 30 bar. The pressure drop across the reactor can aid in the movement of gas and / or carbon particles through the reactor.
[0057] The systems and methods described herein can produce carbon products having a higher carbon-14 to carbon-12 ratio than the same systems using fossil fuel hydrocarbon feedstocks. For example, carbon products produced using fossil fuel feedstocks can have a carbon-14 to carbon-12 ratio of about 3×10 -13 The carbon products described herein can have a carbon-14 to carbon-12 ratio of greater than about 3×10 -13 The carbon products produced by the systems and methods described herein may have a carbon-14 to carbon-12 ratio of greater than 10%. The carbon products produced by the systems and methods described herein may have a carbon-14 ratio of greater than 5% than carbon products produced from a fossil fuel hydrocarbon feedstock.
[0058] The one or more gases (e.g., the feedstock alone or in combination with at least one process gas) may be heated to, for example, about 1,000°C, 1,100°C, 1,200°C, 1,300°C, 1,400°C, 1,500°C, 1,600°C, 1,700°C, 1,800°C, 1,900°C, 2,000°C, 2,050°C, 2,100°C, 2,150°C, 2,200°C, 2,250°C, 2,300°C, 2,350°C, 2,400°C, 2,500°C, 2,600°C, 2,700°C, 2,800°C, 2,900°C, 3,000°C, 3,100°C, 3,200°C, 3,300°C, 3,400°C, 3,500°C, 3,600°C, 3,700°C, 3,800°C, 3,900°C, 4,100°C, 4,100°C, 4,100°C, 4,100°C, 4,200°C, 4,300°C, 4,400°C, 4,500°C, 4,600°C, 4,700°C, 4,800°C, 4,100°C, 4,100°C, 4,200°C, 4,300°C, 4,400°C, 4,500°C, 4,600°C, 4,700°C It may be subjected to (e.g., exposed to) temperatures of 400°C, 2,450°C, 2,500°C, 2,550°C, 2,600°C, 2,650°C, 2,700°C, 2,750°C, 2,800°C, 2,850°C, 2,900°C, 2,950°C, 3,000°C, 3,050°C, 3,100°C, 3,150°C, 3,200°C, 3,250°C, 3,300°C, 3,350°C, 3,400°C, or 3,450°C or greater. Alternatively or additionally, one or more gases (e.g., feedstocks alone or in combination with at least one process gas) may be heated to, for example, about 3,500°C, 3,450°C, 3,400°C, 3,350°C, 3,300°C, 3,250°C, 3,200°C, 3,150°C, 3,100°C, 3,050°C, 3,000°C, 2,950°C, 2,900°C, 2,850°C, 2,800°C, 2,750°C, 2,700°C, 2,650°C, 2,600°C, 2,850°C, 2,8 ...3,100°C, 3,100°C, 3,250°C, 3,200°C, 3,300°C, 3,400°C, 3,500°C, 3,600°C, 3,700°C, 3,800°C, 3,900°C, 4,100°C, 4,100°C, 4,100°C, 4,200°C, 4,200°C, 4,300°C, 4,400°C, 4,500°C, 4,6 The feedstock may be heated and / or subjected to (e.g., exposed to) a temperature of up to 0° C., 2,550° C., 2,500° C., 2,450° C., 2,400° C., 2,350° C., 2,300° C., 2,250° C., 2,200° C., 2,150° C., 2,100° C., 2050° C., 2,000° C., 1,900° C., 1,800° C., 1,700° C., 1,600° C., 1,500° C., 1,400° C., 1,300° C., 1,200° C., or 1,100° C. One or more gases (e.g., the feedstock alone or in combination with at least one process gas) may be heated to such a temperature by a heat generator (e.g., a plasma generator).The one or more gases (e.g., the feedstock, alone or in combination with at least one process gas) may be electrically heated to such a temperature by a heat generator (e.g., the heat generator may be powered by electrical energy). Such a heat generator may have an appropriate power.
[0059] The heat generator can be operated at any suitable power, for example, about 0.5 kilowatts (kW), 1 kW, 1.5 kW, 2 kW, 5 kW, 10 kW, 25 kW, 50 kW, 75 kW, 100 kW, 150 kW, 200 kW, 250 kW, 300 kW, 350 kW, 400 kW, 450 kW, 500 kW, 550 kW, 600 kW, 650 kW, 700 kW, 750 kW, 800 kW, 850 kW, 900 kW, 950 kW, 1 megawatt (MW), 1.05 MW, 1.1 MW, 1.15 MW, 1.2 MW, 1.25 MW, 1.3 MW, 1.35 MW, 1.4 MW, 1.45 MW, 1.5 MW, 1.6 MW, 1.7 MW, 1.8 MW, 1. 9MW, 2MW, 2.5MW, 3MW, 3.5MW, 4MW, 4.5MW, 5MW, 5.5MW, 6MW, 6.5MW, 7MW, 7.5MW, 8MW, 8.5MW, 9MW, 9.5MW, 10MW, 10.5MW, 11MW, 11.5MW, 12MW, 12.5MW, 13MW, 13.5MW, 14MW, 14.5MW, 15MW, 16MW, 17MW, 18MW, 19MW, 20MW, 25MW, 30MW, 35MW, 40MW, 45MW, 50MW, 55MW, 60MW, 65MW, 70MW, 75MW, 80MW, 85MW, 90MW, 95MW or 100MW or more.Alternatively or in addition, the power may be, for example, about 100 MW, 95 MW, 90 MW, 85 MW, 80 MW, 75 MW, 70 MW, 65 MW, 60 MW, 55 MW, 50 MW, 45 MW, 40 MW, 35 MW, 30 MW, 25 MW, 20 MW, 19 MW, 18 MW, 17 MW, 16 MW, 15 MW, 14.5 MW, 14 MW, 13.5 MW, 13 MW, 12.5 MW, 12 MW, 11.5 MW, 11 MW, 10.5 MW, 10 MW, 9.5 MW, 9 MW, 8.5 MW, 8 MW, 7.5 MW, 7 MW, 6.5 MW, 6 MW, 5.5 MW, 5 MW, 4.5 MW, 4 MW, 3.5 MW, 3 MW, W, 2.5 MW, 2 MW, 1.9 MW, 1.8 MW, 1.7 MW, 1.6 MW, 1.5 MW, 1.45 MW, 1.4 MW, 1.35 MW, 1.3 MW, 1.25 MW, 1.2 MW, 1.15 MW, 1.1 MW, 1.05 MW, 1 MW, 950 kW, 900 kW, 850 kW, 800 kW, 750 kW, 700 kW, 650 kW, 600 kW, 550 kW, 500 kW, 450 kW, 400 kW, 350 kW, 300 kW, 250 kW, 200 kW, 150 kW, 100 kW, 75 kW, 50 kW, 25 kW, 10 kW, 5 kW, 2 kW, 1.5 kW or 1 kW or less.
[0060] Carbonaceous materials (e.g., carbon particles) may be produced in, for example, about 1%, 5%, 10%, 25%, 50%, 55%, 60%, 65%, 70%, 75%, 80%, 85%, 90%, 91%, 92%, 93%, 94%, 95%, 96%, 97%, 98%, 99%, 99.5% or 99.9% or greater yields (e.g., yield based on feed conversion, yield based on total hydrocarbons provided, yield based on weight percent carbon, or yield measured by moles of carbon produced versus moles of reactant carbon). Alternatively or additionally, carbonaceous materials (e.g., carbon particles) may be produced in a yield (e.g., yield based on feed conversion, yield based on total hydrocarbons provided, yield based on weight percent carbon, or yield measured by moles of carbon produced versus moles of reactant carbon) of, for example, about 100%, 99.9%, 99.5%, 99%, 98%, 97%, 96%, 95%, 94%, 93%, 92%, 91%, 90%, 85%, 80%, 75%, 70%, 65%, 60%, 55%, 50%, 25%, or 5% or less. The carbon particles may include larger carbon particles. Larger carbon particles may have a spherical equivalent diameter of about 0.5, 0.6, 0.7, 0.75, 0.8, 0.9, 1, 1.1, 1.2, 1.25, 1.3, 1, 4, 1.5, 1.6, 1.7, 1.75, 1.8, 1.9, 2, 2.1, 2.2, 2.25, 2.3, 2.4, 2.5, 2.6, 2.7, 2.75, 2.8, 2.9, 3, 4, 5 micrometers or more, and a spherical equivalent diameter of about 50, 40, 30, 20, 15, 10, 5 meters per square gram (m 2For example, the larger carbon particles may have a spherical equivalent diameter of at least about 2 micrometers and a N2SA of less than about 15 square meters per gram. The larger carbon particles may be captured in a catch pot as described elsewhere herein. The carbon particles may include carbon particles having a spherical equivalent diameter of less than about 5, 4, 3, 2.9, 2.8, 2.75, 2.7, 2.6, 2.5, 2.4, 2.3, 2.25, 2.2, 2.1, 2, 1.9, 1.8, 1.75, 1.7, 1.6, 1.5, 1.4, 1.3, 1.25, 1.2, 1.1, 1, 0.9, 0.8, 0.75, 0.7, 0.6, 0.5, 0.4, 0.3, 0.25, 0.2, 0.1 micrometers or less. For example, the carbon particles can have a spherical equivalent diameter of less than about 2 micrometers. The carbon particles can have a ratio of larger carbon particles (e.g., spherical equivalent diameter greater than about 2 micrometers) to carbon particles with a spherical equivalent diameter of less than about 2 micrometers of about 0 / 100, 5 / 95, 10 / 90, 15 / 85, 20 / 80, 25 / 75, 30 / 70, 35 / 65, 40 / 60, 45 / 55, 50 / 50, 55 / 45, 60 / 40, 65 / 35, 70 / 30, 75 / 25, 80 / 20, 85 / 15, 90 / 10, or 100 / 0. The methods and systems described herein can be configured to be adjusted to produce a predetermined ratio of larger carbon particles to carbon particles with a volume-equivalent sphere of less than about 2 micrometers. The spherical equivalent diameter can be measured by centrifugal particle sedimentation. Further information can be found in "Principles of Colloid and Surface Chemistry" Hiemenz, Rajagopalan, 3rd Edition, pages 70-78, which is incorporated herein by reference in its entirety.
[0061] 5 shows a flow chart of a process 500 for forming carbon particles in a reactor, according to some embodiments. In operation 510, the process 500 can include using one or more electrodes to generate a plasma in the reactor. The carbon particles can be as described elsewhere herein.
[0062] In some cases, the one or more electrodes may include one or more alternating current (AC) electrodes. The AC electrodes may be electrodes configured to operate under AC conditions. For example, the AC electrodes may be electronically coupled to an AC power source and may generate a plasma when an AC current flows through the AC electrodes. In some cases, the one or more electrodes may include one or more direct current (DC) electrodes. The DC electrodes may be configured to operate under DC conditions (e.g., when operably coupled to a DC power source).
[0063] In another operation 520, the process 500 may include injecting a hydrocarbon into a reactor via one or more injectors such that the hydrocarbon contacts the plasma, thereby generating carbon particles. The reactor may be at least approximately 0 bar, 0.5 bar, 1 bar, 1.1 bar, 1.2 bar, 1.3 bar, 1.4 bar, 1.5 bar, 1.6 bar, 1.7 bar, 1.8 bar, 1.9 bar, 2 bar, 2.1 bar, 2.2 bar, 2.3 bar, 2.4 bar, 2.5 bar, 2.6 bar, 2.7 bar, 2.8 bar, 2.9 bar, 3 bar, 3.1 bar, 3.2 bar, 3.3 bar, 3.4 bar, 3.5 bar, 3.6 bar, 3.7 bar, 3.8 bar, 3.9 bar, 4 bar, 5 bar, 6 bar, 7 bar, 8 bar, 9 bar, 10 bar, 11 bar, 12 bar, 13 bar, 14 bar, 15 bar, 16 bar, 17 bar, 18 bar, 19 bar, 20 bar, 21 bar, 22 bar, 23 bar, 24 bar, 25 bar, 26 bar, 27 bar, 28 bar, 29 bar, 30 bar, 31 bar, 32 bar, 33 bar, 34 bar, 35 bar, 36 bar, 37 bar, 38 bar, 39 bar, 40 bar, 41 bar, 42 bar, 43 bar, 44 bar, 45 bar, 46 bar, 47 bar, 48 bar, 49 bar, 50 bar, 51 bar, 52 bar, 53 bar, 54 bar, 55 bar, 56 bar, 57 bar, 58 bar, 59 bar, , 4.5 bar, 5 bar, 6 bar, 7 bar, 8 bar, 9 bar, 10 bar, 11 bar, 12 bar, 13 bar, 14 bar, 15 bar, 16 bar, 17 bar, 18 bar, 19 bar, 20 bar, 21 bar, 22 bar, 23 bar, 24 bar, 25 bar, 26 bar, 27 bar, 28 bar, 29 bar, 30 bar, 35 bar, 40 bar, 45 bar, 50 bar, 55 bar, 60 bar, 65 bar, 70 bar, 75 bar or more.The reactor can operate at up to approximately 100bar, 90bar, 80bar, 75bar, 70bar, 65bar, 60bar, 55bar, 50bar, 45bar, 40bar, 35bar, 30bar, 29bar, 28bar, 27bar, 26bar, 25bar, 24bar, 23bar, 22bar, 21bar, 20bar, 19bar, 18bar, 17bar, 16bar, 15bar, 14bar, 13bar, 12bar, 11bar, 10bar, 9bar, 8bar, 7bar, 6bar , 5 bar, 4 bar, 3.9 bar, 3.8 bar, 3.7 bar, 3.6 bar, 3.5 bar, 3.4 bar, 3.3 bar, 3.2 bar, 3.1 bar, 3 bar, 2.9 bar, 2.8 bar, 2.7 bar, 2.6 bar, 2.5 bar, 2.4 bar, 2.3 bar, 2.2 bar, 2.1 bar, 2 bar, 1.9 bar, 1.8 bar, 1.7 bar, 1.6 bar, 1.5 bar, 1.4 bar, 1.3 bar, 1.2 bar, 1.1 bar or less. The reactor can be operated at a pressure within a range defined by any two of the proceeding values. For example, the reactor can be operated at a pressure within a range of about 1.1 bar to about 4 bar.
[0064] In some cases, the process 500 can produce hydrogen. For example, in the production of carbon particles, hydrogen gas can also be produced. The hydrogen can be discarded (e.g., disposed as waste from the process). The hydrogen can be collected (e.g., as a further product of the process). The hydrogen and carbon particles can be produced in a once-through, single-stage process. For example, hydrogen and carbon particles can be produced simultaneously (e.g., the process operation that produces the carbon particles can also produce hydrogen). In this example, the hydrogen and carbon particles can be produced in a single run of the reactor (e.g., the same hydrocarbon cracking operation). The single-stage process can increase the reaction efficiency (e.g., efficiency of heat transfer from the plasma to the feedstock). Additionally, the single-stage process can provide a higher plasma temperature. For example, the plasma in a single-stage process can be at a temperature of about 3500 to about 4000° C. The single-stage process can have a thermal gradient between the center of the reactor and the walls of the reactor. The thermal gradient between the center of the reactor and the walls of the reactor can be smaller in a single-stage process than in a multi-stage process. For example, the thermal gradient in a single stage process can be from a center temperature of 3500 degrees Celsius to a wall temperature of about 1800 degrees Celsius, while a two stage process can have a center temperature of about 3500 degrees Celsius and a wall temperature of about 2200 to 2400 degrees Celsius. A single stage process can allow for cost savings due to the types of materials of construction and maintenance possible. For example, lower temperatures near the walls of the reactor can allow lower cost materials to be used in the construction of the reactor and can reduce thermal wear on the walls of the reactor. A single stage reactor can have a high density (e.g., optically dense) field of carbon particles in or near the plasma arc (e.g., as described elsewhere herein). Such a high density field can increase heat transfer to the carbon particles and decrease heat transfer to the walls of the reactor.
[0065] In some cases, hydrogen and carbon particles can be produced in a multi-stage (e.g., two-stage, three-stage, etc.) process. For example, a two-stage process can include a first injection of a hydrocarbon and a second injection of a hydrocarbon. The use of a multi-stage process can reduce fouling in the reactor or on the electrodes by reducing the amount of hydrocarbons in a given area of the reactor. Multiple stages can also allow additional process operations to occur between stages. For example, water injection can be performed to remove fouling from the reactor without having to shut down the reactor or disable the plasma. Multiple stages can also increase mixing of the feedstock into the plasma gas due to increased velocity and momentum of the plasma gas.
[0066] The plasma reactor of the present disclosure may operate at temperatures of at least about 1000, 1100, 1200, 1300, 1400, 1500, 1600, 1700, 1800, 1900, 2000, 2100, 2200, 2300, 2400, 2500, 2600, 2700, 2800, 2900, 3000, 3100, 3200, 3300, 3400, 3500, 3600, 3700, 3800, 3900, 4000, 4100, 4200, 4300, 4400, 4500 degrees Celsius or greater. The plasma reactor of the present disclosure can operate at temperatures up to about 4500, 4400, 4300, 4200, 4100, 4000, 3900, 3800, 3700, 3600, 3500, 3400, 3300, 3200, 3100, 3000, 2900, 2800, 2700, 2600, 2500, 2400, 2300, 2200, 2100, 2000, 1900, 1800, 1700, 1600, 1500, 1400, 1300, 1200, 1100, 1000 degrees Celsius or less. The plasma reactor of the present disclosure can operate at a temperature range defined by any two of the progression values. For example, the plasma reactor can operate at a temperature of about 3500 degrees Celsius to about 4000 degrees Celsius. The temperature gradient between the center of the reactor of the present disclosure and the walls of the reactor can be at least about 50, 100, 200, 300, 400, 500, 600, 700, 800, 900, 1000, 1100, 1200, 1300, 1400, 1500, 1600, 1700, 1800, 1900, 2000 degrees Celsius or more. For example, the temperature difference between the center of the reactor and the walls of the reactor can be at least about 1700 degrees Celsius. The temperature gradient between the center of the reactor and the wall of the reactor of the present disclosure may be up to about 2000, 1900, 1800, 1700, 1600, 1500, 1400, 1300, 1200, 1100, 1000, 900, 800, 700, 600, 500, 400, 300, 200, 100, 50 degrees Celsius or less difference. The temperature gradient between the center of the reactor and the wall of the reactor of the present disclosure may be defined by any two ranges of progression values. The magnitude of the gradient may be related to the type of reactor system used. For example, a single stage reactor may provide a larger temperature gradient than a multi-stage reactor.
[0067] In some cases, the systems and methods described herein produce 1 ton of hydrogen per hour. The hydrogen produced can be purified to a given purity, for example, 90%, 95%, 99%, 99.5%, or 99.9%. In some cases, the hydrogen is produced at a rate of about 0.1 ton / hour to about 10 ton / hour. In some cases, the hydrogen is produced at a rate of about 0.1 ton / hour to about 0.5 ton / hour, about 0.1 ton / hour to about 1 ton / hour, about 0.1 ton / hour to about 5 ton / hour, about 0.1 ton / hour to about 10 ton / hour, about 0.5 ton / hour to about 1 ton / hour, about 0.5 ton / hour to about 5 ton / hour, about 0.5 ton / hour to about 10 ton / hour, about 1 ton / hour to about 5 ton / hour, about 1 ton / hour to about 10 ton / hour, or about 5 ton / hour to about 10 ton / hour. In some cases, hydrogen is produced at a rate of about 0.1 ton / hour, about 0.5 ton / hour, about 1 ton / hour, about 5 ton / hour, or about 10 ton / hour. In some cases, hydrogen is produced at a rate of at least about 0.1 ton / hour, about 0.5 ton / hour, about 1 ton / hour, or about 5 ton / hour. In some cases, hydrogen is produced at a rate of up to about 0.5 ton / hour, about 1 ton / hour, about 5 ton / hour, or about 10 ton / hour.
[0068] The hydrocarbon may be as described elsewhere herein. For example, the hydrocarbon may be a gas (e.g., including natural gas). The hydrocarbon may be heated upon contact with the plasma. For example, interaction of the hydrocarbon with the plasma may result in imparting energy from the plasma to the hydrocarbon, thereby heating the hydrocarbon. The hydrocarbon may be decomposed (e.g., at least partially decomposed) upon contact with the plasma.
[0069] The carbon particles may have a smaller surface area than carbon particles formed in a reactor operated at a lower pressure than the reactor of process 500. For example, if the reactor of process 500 is operated at a pressure of 1.5 bar, the carbon particles produced by the reactor operated at a pressure of 1.5 bar may have a smaller surface area than carbon particles formed in the same reactor operated at a pressure of 2.5 bar. In another example, if the reactor of process 500 is operated at a pressure of 5 bar, the carbon particles produced by the reactor operated at a pressure of 5 bar may have a smaller surface area than carbon particles formed in the same reactor operated at a pressure of 3 bar. The carbon particles can have a surface area that is at least about 5, 10, 15, 20, 25, 30, 35, 40, 45, 50, 55, 60, 65, 70, 75, 80, 81, 82, 83, 84, 85, 86, 87, 88, 89, 90, 91, 92, 93, 94, 95, 96, 97, 98, 99, 99.9 percent or more of the surface area of the carbon particles formed in the reactor when the reactor is operated at a pressure lower than the pressure of the reactor of process 500 (e.g., less than about 1.5 bar, less than about 5 bar, less than about 10 bar, etc.). The carbon particles may have a surface area of up to about 99.9, 99, 98, 97, 96, 95, 94, 93, 92, 91, 90, 89, 88, 87, 86, 85, 84, 83, 82, 81, 80, 75, 70, 65, 60, 55, 50, 45, 40, 35, 30, 25, 20, 15, 10, 5 or less percent of the surface area of the carbon particles formed in the reactor when the reactor is operated at a pressure lower than the pressure of the reactor of process 500 (e.g., less than about 1.5 bar, less than about 5 bar, less than about 10 bar, etc.).
[0070] The surface area of the carbon particles can be increased using one or more additives. The one or more additives may be added to the hydrocarbon before, during, or after the hydrocarbon is injected into the reactor. The one or more additives may be injected into the reactor before the plasma. Examples of additives include, but are not limited to, hydrocarbons (e.g., hydrocarbons described elsewhere herein, hydrocarbon gases), silicon-containing compounds (e.g., siloxanes, silanes, etc.), aromatic additives (e.g., benzene, xylene, polycyclic aromatic hydrocarbons, etc.), and the like, or any combination thereof. The reactor may be an oxygen-free environment. The oxygen-free environment may be an unbound oxygen-free environment. For example, the reactor may be substantially free of unbound oxygen (e.g., elemental oxygen), but may include bound oxygen (e.g., as part of ethanol, carbon dioxide, etc.). The reactor may contain less than up to about 20, 15, 14, 13, 12, 11, 10, 9, 8, 7, 6, 5, 4, 3, 2, 1, 0.5, 0.1, 0.05, 0.01, 0.005, 0.001, 0.0005, 0.0001 percent molecular oxygen or molar percent.
[0071] The carbon particles may include carbon black. Examples of carbon particles include, but are not limited to, carbon black, coke, needle coke, graphite, macrocyclic polycyclic aromatic hydrocarbons, activated carbon, and the like, or any combination thereof. The carbon particles may be produced by the process 500 in a yield greater than the yield of carbon particles formed by the reactor when operated at a pressure lower than the pressure of the process 500 (e.g., less than about 1 bar, about 1.5 bar, etc.). The carbon particles may be produced in a percent yield of at least about 5, 10, 15, 20, 25, 30, 35, 40, 45, 50, 55, 60, 65, 70, 75, 80, 81, 82, 83, 84, 85, 86, 87, 88, 89, 90, 91, 92, 93, 94, 95, 96, 97, 98, 99, 99.9, or more. The carbon particles may be produced in a yield of up to about 99.9, 99, 98, 97, 96, 95, 94, 93, 92, 91, 90, 89, 88, 87, 86, 85, 84, 83, 82, 81, 80, 75, 70, 65, 60, 55, 50, 45, 40, 35, 30, 25, 20, 15, 10, 5 percent or less. The yield of carbon particles may be a value within any two of the proceeding values. For example, the yield of carbon particles may be about 90 to about 99%. The yield of carbon particles in process 500 may be greater than the yield of carbon particles formed in a different reactor of the same size as the reactor of process 500 if the different reactor is operated at a pressure lower than the pressure of the reactor of process 500.
[0072] FIG. 6 shows a flow chart of a process 600 for generating hydrogen in a reactor, according to some embodiments. In operation 610, the process 600 can include using one or more electrodes to generate a plasma in the reactor. In some cases, the one or more electrodes can include one or more alternating current (AC) electrodes. The AC electrodes can be electrodes configured to operate under AC conditions. For example, the AC electrodes can be electronically coupled to an AC power source and can generate a plasma when an AC current flows through the AC electrodes. In some cases, the one or more electrodes can include one or more direct current (DC) electrodes. The DC electrodes can be configured to operate under DC conditions (e.g., when operably coupled to a DC power source).
[0073] In some cases, the systems and methods described herein produce 1 ton of hydrogen per hour. The hydrogen produced can be purified to a given purity, for example, 90%, 95%, 99%, 99.5%, or 99.9%. In some cases, the hydrogen is produced at a rate of about 0.1 ton / hour to about 10 ton / hour. In some cases, the hydrogen is produced at a rate of about 0.1 ton / hour to about 0.5 ton / hour, about 0.1 ton / hour to about 1 ton / hour, about 0.1 ton / hour to about 5 ton / hour, about 0.1 ton / hour to about 10 ton / hour, about 0.5 ton / hour to about 1 ton / hour, about 0.5 ton / hour to about 5 ton / hour, about 0.5 ton / hour to about 10 ton / hour, about 1 ton / hour to about 5 ton / hour, about 1 ton / hour to about 10 ton / hour, or about 5 ton / hour to about 10 ton / hour. In some cases, hydrogen is produced at a rate of about 0.1 ton / hour, about 0.5 ton / hour, about 1 ton / hour, about 5 ton / hour, or about 10 ton / hour. In some cases, hydrogen is produced at a rate of at least about 0.1 ton / hour, about 0.5 ton / hour, about 1 ton / hour, or about 5 ton / hour. In some cases, hydrogen is produced at a rate of up to about 0.5 ton / hour, about 1 ton / hour, about 5 ton / hour, or about 10 ton / hour.
[0074] In another operation 620, the process 600 may include injecting hydrocarbons into a reactor via one or more injectors such that the hydrocarbons contact the plasma and thereby produce hydrogen. The reactor may be at least approximately 0 bar, 0.5 bar, 1 bar, 1.1 bar, 1.2 bar, 1.3 bar, 1.4 bar, 1.5 bar, 1.6 bar, 1.7 bar, 1.8 bar, 1.9 bar, 2 bar, 2.1 bar, 2.2 bar, 2.3 bar, 2.4 bar, 2.5 bar, 2.6 bar, 2.7 bar, 2.8 bar, 2.9 bar, 3 bar, 3.1 bar, 3.2 bar, 3.3 bar, 3.4 bar, 3.5 bar, 3.6 bar, 3.7 bar, 3.8 bar, 3.9 bar, 4 bar, 5 bar, 6 bar, 7 bar, 8 bar, 9 bar, 10 bar, 11 bar, 12 bar, 13 bar, 14 bar, 15 bar, 16 bar, 17 bar, 18 bar, 19 bar, 20 bar, 21 bar, 22 bar, 23 bar, 24 bar, 25 bar, 26 bar, 27 bar, 28 bar, 29 bar, 30 bar, 31 bar, 32 bar, 33 bar, 34 bar, 35 bar, 36 bar, 37 bar, 38 bar, 39 bar, 40 bar, 41 bar, 42 bar, 43 bar, 44 bar, 45 bar, 46 bar, 47 bar, 48 bar, 49 bar, 50 bar, 51 bar, 52 bar, 53 bar, 54 bar, 55 bar, 56 bar, 57 bar, 58 bar, 59 bar, 6 , 4.5 bar, 5 bar, 6 bar, 7 bar, 8 bar, 9 bar, 10 bar, 11 bar, 12 bar, 13 bar, 14 bar, 15 bar, 16 bar, 17 bar, 18 bar, 19 bar, 20 bar, 21 bar, 22 bar, 23 bar, 24 bar, 25 bar, 26 bar, 27 bar, 28 bar, 29 bar, 30 bar, 35 bar, 40 bar, 45 bar, 50 bar, 55 bar, 60 bar, 65 bar, 70 bar, 75 bar or more.The reactor can operate at up to approximately 100bar, 90bar, 80bar, 75bar, 70bar, 65bar, 60bar, 55bar, 50bar, 45bar, 40bar, 35bar, 30bar, 29bar, 28bar, 27bar, 26bar, 25bar, 24bar, 23bar, 22bar, 21bar, 20bar, 19bar, 18bar, 17bar, 16bar, 15bar, 14bar, 13bar, 12bar, 11bar, 10bar, 9bar, 8bar, 7bar, 6bar , 5 bar, 4 bar, 3.9 bar, 3.8 bar, 3.7 bar, 3.6 bar, 3.5 bar, 3.4 bar, 3.3 bar, 3.2 bar, 3.1 bar, 3 bar, 2.9 bar, 2.8 bar, 2.7 bar, 2.6 bar, 2.5 bar, 2.4 bar, 2.3 bar, 2.2 bar, 2.1 bar, 2 bar, 1.9 bar, 1.8 bar, 1.7 bar, 1.6 bar, 1.5 bar, 1.4 bar, 1.3 bar, 1.2 bar, 1.1 bar or less. The reactor can be operated at a pressure within a range defined by any two of the proceeding values. For example, the reactor can be operated at a pressure within a range of about 1.1 bar to about 4 bar.
[0075] In some cases, the process 600 further includes producing carbon particles. The carbon particles may be as described elsewhere herein. For example, the carbon particles may be produced simultaneously in the course of producing hydrogen. The process may include continuously producing the hydrogen and carbon particles. For example, the hydrogen and carbon particles may be produced continuously (e.g., not a batch process). The hydrogen and carbon particles may be produced in a once-through, single-stage process, as described elsewhere herein.
[0076] In some cases, the hydrocarbon is as described elsewhere herein. For example, the hydrocarbon can include natural gas. The hydrocarbon can be heated upon contact with the plasma, as described elsewhere herein. In some cases, the reactor is an oxygen-free environment, as described elsewhere herein. For example, the reactor can include less than about 2% molecular oxygen by volume or mole.
[0077] FIG. 10 is an example of a high-pressure degasser 1000 according to some embodiments. Carbon particles (e.g., carbon black, etc.) produced by methods described elsewhere herein can be directed to the top of the degasser as shown. The carbon particles can first contact a filter prior to the high-pressure degasser and fall from the filter to the top of the device as shown. The carbon particles can contact a rotary valve 1001. The rotary valve can be configured to meter the carbon particles by dropping them through an open airlock valve 1002 into a degassing vessel 1003. The presence of the rotary valve can prevent too many carbon particles from entering the degassing vessel at once. The rotary valve can also provide a certain amount of backflow protection against gas from the degassing vessel backflowing. The carbon particles can be collected in the degassing vessel until a predetermined amount of carbon particles is reached. The rotary valve 1001 and airlock valve 1002 can then be closed and the vent valve 1005 can be opened. The vent valve opening can release gas at pressure within the degassing vessel (e.g., if carbon particles are introduced into the vessel under pressure) and place the degassing vessel at atmospheric pressure. The vent valve can then be closed and the inert purge valve 1004 can be opened to allow the flow of an inert gas (e.g., an inert gas as described elsewhere herein). The inert gas can be configured to displace and / or dilute gas associated with (e.g., adsorbed) the carbon particles. For example, flammable and / or explosive gases (e.g., hydrogen, hydrocarbons, etc.) can be adsorbed onto the surface of the carbon particles and the inert gas can displace the flammable and / or explosive gas. Following introduction of the inert gas, the purge valve 1004 can be closed and the vent valve 1005 can be opened to vent a mixture of the inert gas and gas associated with the carbon particles. Purging with the inert gas can be repeated until the carbon particles are deemed inert (e.g., gas within the carbon particles is present at a safe level). The carbon particles can then be removed from the degassing vessel via the airlock valve 1006. For example, the airlock valve can be opened and the carbon particles can fall out of the degassing vessel by gravity.The airlock valve 1006 can then be closed and the process repeated with another batch of carbon particles.
[0078] The use of a high pressure degasser may allow for the collection of gases associated with the carbon particles (e.g., hydrogen) at high pressure. For example, hydrogen adsorbed in the pores of the carbon particles can be collected at the same high pressure at which the reactor system is operated. Collecting the gas at high pressure allows for the gas to be used in high pressure systems (e.g., high pressure chemical synthesis, combustion, fuel cells, etc.) without the use of a secondary pressurization device. Thus, the gas can be more easily used in downstream processes due to the high pressure of the gas. This can reduce engineering requirements and improve the functioning of the system compared to when the gas is at a lower pressure.
[0079] In a non-limiting example, a reactor according to the present disclosure can provide an energy input of 19 megawatts and a natural gas feed flow of 5.7 tons / hour. In this example, a 10 kilogram / hour purge of inert gas (e.g., argon) can be fed with a 50 kilogram / hour recycle gas flow (e.g., containing 40% H2, 10% natural gas, 10% ethylene, 10% ethane, 10% other hydrocarbons, traces of HCN, 20% Ar, 10% CO, or any combination of these percentages). In this example, about 1.25 tons / hour of hydrogen can be produced and about 3.5 tons / hour of carbon particles can be produced. In this example, an electrode wear rate of about 8 kilograms per ton of carbon particles can be observed.
[0080] In another non-limiting example, a two-stage atmospheric pressure reactor can be contrasted with the high pressure reactor of the present disclosure. The atmospheric reactor can be supplied with 18 megawatts of energy, 3 tons / hour of natural gas feed, and 300 kilograms of recycled hydrogen. In this example, only 0.75 tons / hour of hydrogen can be produced using 2 tons / hour of carbon particles with a similar carbon particle electrode wear of 8 kilograms / ton. As shown by this example, the increased pressure of the present disclosure can provide capital cost savings and improved efficiency compared to a two-stage atmospheric reactor.
[0081] The systems and methods of the present disclosure may be implemented in any manner similar to those disclosed in U.S. Patent Application Publication No. 2015 / 0210856 and WO 2015 / 116807 ("System for High Temperature Chemical Processing"), U.S. Patent Application Publication No. 2015 / 0211378 ("Integration of Plasma and Hydrogen Processes with Combined Cycle Power Plants, Simple Cycle Power Plants and Steam Reformers"), WO 2015 / 116797 ("Integration of Plasma and Hydrogen Processes with Combined Cycle Power Plants and Steam Reformers"), each of which is incorporated herein by reference in its entirety. No. 2015 / 0210857 and WO 2015 / 116798 ("Use of Feedstock in Carbon Black Plasma Processing"), U.S. Patent Application Publication No. 2015 / 0210858 and WO 2015 / 116800 ("Plasma Gas Throat Assemblies and Methods"), U.S. Patent Application Publication No. 2015 / 0218383 and WO 2015 / 116811 ("Plasma Reactors"), U.S. Patent Application Publication No. 2015 / 0223314 and WO 2015 / 116943 ("Plasma Torch Designs") ), WO 2016 / 126598 ("Carbon Black Combustible Gas Separation"), WO 2016 / 126599 ("Carbon Black Production System"), WO 2016 / 126600 ("Regenerative Cooling Method and Apparatus"), U.S. Patent Application Publication Nos. 2017 / 0034898 and 2017 / 019683 ("DC Plasma Torch Power Design Method and Apparatus"), U.S. Patent Application Publication Nos. 2017 / 0037253 and 2017 / 027385 ("Method of Producing Carbon Black ... No. 2017 / 0058128 and WO 2017 / 034980 ("High Temperature Heat Integration Method for Carbon Black Production"), U.S. Patent Application Publication No. 2017 / 0066923 and WO 2017 / 044594 ("Circular Shaped FEW Layer Graph"), U.S. Patent Application Publication No. 20170073522 and WO 2017 / 048621 ("Carbon Black from Natural Gas"), WO 2017 / 190045 ("Secondary Heat Addition to Particle Production Process and Apparatus"), WO 2017 / 190015 ("Torch Stinger Method and Apparatus"),It may also be combined with or modified by other systems and / or methods (with appropriate mutatis mutandis) such as the chemical processing and heating methods, chemical processing systems, reactors and plasma torches described in WO 2018 / 165483 ("Systems and methods for producing carbon particles using a heat transfer gas"), WO 2018 / 195460 ("Particle systems and methods"), WO 2019 / 046322 ("Particle systems and methods"), WO 2019 / 046320 ("Systems and methods for particle generation"), WO 2019 / 046324 ("Particle systems and methods"), WO 2019 / 084200 ("Particle systems and methods"), and WO 2019 / 195461 ("Systems and methods for processing").
[0082] Computer Systems The present disclosure provides a computer system programmed to perform the methods of the present disclosure. Figure 9 shows a computer system 901 programmed or otherwise configured to perform the methods of the present disclosure, such as a method for forming carbon particles and / or hydrogen. The computer system 901 can coordinate various aspects of the present disclosure, such as the operation of a reactor. The computer system 901 can be a user's electronic device or a computer system located remotely relative to the electronic device. The electronic device can be a mobile electronic device.
[0083] The computer system 901 includes a central processing unit (CPU, also referred to herein as "processor" and "computer processor") 905, which may be a single-core or multi-core processor, or multiple processors for parallel processing. The computer system 901 also includes memory or storage locations 910 (e.g., random access memory, read-only memory, flash memory), an electronic storage unit 915 (e.g., hard disk), a communication interface 920 (e.g., network adapter) for communicating with one or more other systems, and peripherals 925, such as cache, other memory, data storage, and / or electronic display adapters. The memory 910, the storage unit 915, the interface 920, and the peripherals 925 are in communication with the CPU 905 via a communication bus (solid lines), such as a motherboard. The storage unit 915 may be a data storage unit (or data repository) for storing data. The computer system 901 may be operatively coupled to a computer network ("network") 930 with the aid of the communication interface 920. The network 930 can be the Internet, an Internet and / or an extranet, or an intranet and / or an extranet in communication with the Internet. The network 930 is possibly a remote communication and / or data network. The network 930 can include one or more computer servers, which can enable distributed computing, such as cloud computing. The network 930 can possibly implement a peer-to-peer network with the aid of the computer system 901, which allows devices coupled to the computer system 901 to operate as clients or servers.
[0084] The CPU 905 may execute a series of machine-readable instructions, which may be embodied in a program or software. The instructions may be stored in a memory location, such as the memory 910. The instructions may be directed to the CPU 905, which may then program or otherwise configure the CPU 905 to perform the methods of the present disclosure. Examples of operations performed by the CPU 905 may include fetch, decode, execute, and writeback.
[0085] The CPU 905 may be part of a circuit, such as an integrated circuit. One or more other components of the system 901 may be included in the circuit. In some cases, the circuit is an application specific integrated circuit (ASIC).
[0086] The storage unit 915 can store files such as drivers, libraries, and saved programs. The storage unit 915 can store user data, such as user preferences and user programs. The computer system 901 can optionally include one or more additional data storage units external to the computer system 901, such as located on a remote server in communication with the computer system 901 via an intranet or the Internet.
[0087] The computer system 901 can communicate with one or more remote computer systems via the network 930. For example, the computer system 901 can communicate with a remote computer system of a user. Examples of remote computer systems include a personal computer (such as a portable PC), a slate or tablet PC (e.g., Apple® iPad®, Samsung® Galaxy Tab), a phone, a smartphone (e.g., Apple® iPhone®, Android-enabled device, Blackberry®), or a personal digital assistant. A user can access the computer system 901 via the network 930.
[0088] The methods herein may be implemented by machine (e.g., computer processor) executable code stored in an electronic storage location of the computer system 901, such as, for example, memory 910 or electronic storage unit 915. The machine executable or machine readable code may be provided in the form of software. In use, the code may be executed by the processor 905. In some cases, the code may be retrieved from the storage unit 915 and stored in the memory 910 for immediate access by the processor 905. In some circumstances, the electronic storage unit 915 may be eliminated and machine executable instructions are stored in the memory 910.
[0089] The code may be pre-compiled and configured for use on a machine having a processor adapted to execute the code, or it may be compiled at run-time. The code may be provided in a programming language that may be selected to allow the code to be executed in a pre-compiled or compiled manner.
[0090] Aspects of the systems and methods provided herein, such as computer system 901, may be embodied in programming. Various aspects of the technology may be considered as "products" or "articles of manufacture" generally in the form of machine (or processor) executable code and / or associated data held or embodied in some type of machine-readable medium. The machine executable code may be stored in an electronic storage unit such as a memory (e.g., read-only memory, random access memory, flash memory) or a hard disk. A "storage" type medium may include any or all of the tangible memory of a computer, processor, etc., or associated modules such as various semiconductor memories, tape drives, disk drives, etc., that may provide persistent storage at any time for software programming. All or a portion of the software may be communicated over the Internet or various other communication networks. Such communication may enable, for example, loading of the software from one computer or processor to another, for example, from a management server or host computer to a computer platform of an application server. Thus, other types of media that may bear software elements include optical, electrical, and electromagnetic waves, such as those used across physical interfaces between local devices, via wired and optical land line networks, and across various air links. The physical elements that convey such waves, such as wired or wireless links, optical links, etc., may also be considered media bearing software. As used herein, terms such as computer or machine "readable medium" refer to any medium that participates in providing instructions to a processor for execution, unless limited to persistent, tangible "storage" media.
[0091] Thus, a machine-readable medium such as a computer-executable code may take many forms, including but not limited to a tangible storage medium, a carrier wave medium, or a physical transmission medium. Non-volatile storage media include optical or magnetic disks, such as any storage device of any computer(s) such as may be used to implement, for example, the databases shown in the figures. Volatile storage media include dynamic memory such as the main memory of such a computer platform. Tangible transmission media include coaxial cables, copper wire and optical fibers, including the wiring that comprises a bus within a computer system. Carrier wave transmission media may take the form of electric or electromagnetic signals, or acoustic or light waves such as those generated during radio frequency (RF) and infrared (IR) data communications. Thus, common forms of computer readable media include, for example, floppy disks, flexible disks, hard disks, magnetic tape, other magnetic media, CD-ROMs, DVDs or DVD-ROMs, any other optical media, punch cards paper tape, any other physical storage media with a pattern of holes, RAM, ROM, PROMs and EPROMs, FLASH-EPROMs, any other memory chips or cartridges, carrier waves transmitting data or instructions, cables or links transmitting such waves, or any other medium from which a computer can read programming code and / or data. Many of these forms of computer readable media may be involved in carrying one or more sequences of one or more instructions to a processor for execution.
[0092] The computer system 901 may include or communicate with, for example, an electronic display 935 with a user interface (UI) 940 for accessing controls for operating the reactor. Examples of UIs include, but are not limited to, graphical user interfaces (GUIs) and web-based user interfaces.
[0093] The methods and systems of the present disclosure may be implemented by one or more algorithms. The algorithms may be implemented via software when executed by the central processing unit 905. The algorithms may, for example, cause the reactor system to operate at least partially autonomously.
[0094] Exemplary embodiments of the present disclosure 1. A process comprising the step of producing hydrogen by heating a hydrocarbon at greater than atmospheric pressure using a plasma generator.
[0095] 2. The method of embodiment 1, further comprising the step of adding a hydrocarbon to the plasma generator.
[0096] 3. The method of embodiment 1, wherein the plasma generator comprises an AC electrode.
[0097] 4. The method of embodiment 1, wherein the plasma generator comprises a DC electrode.
[0098] 5. The method of embodiment 1, further comprising the step of producing a carbonaceous material.
[0099] 6. The method of embodiment 5, wherein the carbonaceous material comprises carbon particles.
[0100] 7. The method of embodiment 5, further comprising the step of continuously producing hydrogen and carbonaceous material.
[0101] 8. The method of embodiment 1, wherein the hydrocarbon is a gas.
[0102] 9. The method of embodiment 1, wherein the hydrocarbon comprises natural gas.
[0103] 10. The method of embodiment 9, wherein the hydrocarbon is natural gas.
[0104] 11. The method of embodiment 5, further comprising heating the hydrocarbon to produce hydrogen in the single chamber.
[0105] 12. The method of embodiment 5, further comprising producing hydrogen and carbonaceous materials in a once-through, single-step process.
[0106] 13. The method of embodiment 5, wherein the pressure is greater than or equal to about 2 bar.
[0107] 14. The method of embodiment 18, wherein the pressure is greater than or equal to about 5 bar.
[0108] 15. The method of embodiment 19, wherein the pressure is greater than or equal to about 10 bar.
[0109] 16. A process comprising the step of producing hydrogen in a substantially inert or substantially oxygen-free environment or atmosphere by heating a hydrocarbon with electrical energy at a pressure greater than atmospheric pressure.
[0110] 17. The method of embodiment 16, further comprising the step of producing a carbonaceous material.
[0111] 18. The method of embodiment 17, wherein the carbonaceous material comprises carbon particles.
[0112] 19. The method of embodiment 17, further comprising the step of continuously producing hydrogen and carbonaceous material.
[0113] 20. The method of embodiment 16, wherein the hydrocarbon is a gas.
[0114] 21. The method of embodiment 16, wherein the hydrocarbon comprises natural gas.
[0115] 22. The method of embodiment 21, wherein the hydrocarbon is natural gas.
[0116] 23. The method of embodiment 16, further comprising the step of heating the hydrocarbon with a plasma generator.
[0117] 24. The method of embodiment 16, further comprising the step of directly heating the hydrocarbon with electrical energy.
[0118] 25. The method of embodiment 16, further comprising producing hydrogen in a refractory-lined reactor.
[0119] 26. The method of embodiment 16, further comprising heating the hydrocarbon to produce hydrogen in the single chamber.
[0120] 27. The method of embodiment 16, further comprising producing hydrogen and carbonaceous materials in a once-through, single-step process.
[0121] 28. The method of embodiment 16, further comprising removing hydrogen from the hydrocarbon using electrical energy.
[0122] 29. The method of embodiment 16, wherein the pressure is about 2 bar or more.
[0123] 30. The method of embodiment 29, wherein the pressure is about 5 bar or more.
[0124] 31. The method of embodiment 30, wherein the pressure is greater than or equal to about 10 bar.
[0125] 32. The method of embodiment 16, further comprising using a heat exchanger, a filter, and solid handling equipment.
[0126] 33. The method of embodiment 32, wherein the solids handling equipment includes a cooled solids carbon collection screw conveyor, an airlock and purge system, a pneumatic conveying system, a mechanical conveying system, a classifying mill, and a product storage vessel.
[0127] 34. The method of embodiment 16, further comprising producing hydrogen in a substantially oxygen-free environment or atmosphere.
[0128] 35. The method of embodiment 16, further comprising generating hydrogen in a substantially inert environment or atmosphere.
[0129] 36. A process comprising the step of producing hydrogen in a substantially inert or substantially oxygen-free environment or atmosphere by directly heating a hydrocarbon with electrical energy.
[0130] 37. The method of embodiment 36, wherein the hydrocarbon is a gas.
[0131] 38. The method of embodiment 36, wherein the hydrocarbon comprises natural gas.
[0132] 39. The method of embodiment 38, wherein the hydrocarbon is natural gas.
[0133] 40. The method of embodiment 36, further comprising the step of producing a carbonaceous material.
[0134] 41. The method of embodiment 40, wherein the carbonaceous material comprises carbon particles.
[0135] 42. The method of embodiment 40, further comprising the step of continuously producing hydrogen and carbonaceous material.
[0136] 43. The method of embodiment 36, further comprising the step of generating a plasma.
[0137] 44. The method of embodiment 43, further comprising generating the plasma using an AC electrode.
[0138] 45. The method of embodiment 43, further comprising generating the plasma using a DC electrode.
[0139] 46. The method of embodiment 36, further comprising generating hydrogen in an environment or atmosphere containing less than about 2% molecular oxygen by volume or molar.
[0140] 47. The method of embodiment 36, further comprising the step of directly heating the hydrocarbon to produce hydrogen in the single chamber.
[0141] 48. The method of embodiment 36, further comprising producing hydrogen and carbonaceous material in a once-through, single-step process.
[0142] 49. A device comprising a reactor configured to operate at an input power of about 10 megawatts to generate a thermal plasma in a confined space, the reactor operating at a pressure of at least about 1.5 bar, a temperature of the reactor wall being less than about 2000°C, and a distance from the center of the reactor to the reactor wall being less than about 3 meters.
[0143] 50. The device of embodiment 49, wherein during use, the reactor comprises a temperature gradient between the center of the reactor and the wall of the reactor.
[0144] 51. The device of embodiment 50, wherein the gradient is formed at least in part due to the use of a hydrocarbon as at least a portion of the plasma gas in the reactor.
[0145] 52. The device of embodiment 51, wherein the gradient of the reactor is at least about 10% greater than a reactor that does not have a hydrocarbon used as at least a portion of the plasma gas.
[0146] The following examples are illustrative of the particular systems and methods described herein and are not intended to be limiting.
[0147] Example 1 - Predicted properties of the ambient pressure reactor described above 7 is a plot of an example of a range of reactor pressures versus normalized surface area measurements, according to one embodiment. The conditions used in this example production can be the use of a plug flow reactor at 1900 K with methane, hydrogen, and nitrogen as process gases.
[0148] The plot shows that as reactor pressure increases, the expected surface area of carbon particles formed in the reactor decreases, the extent of which may be related to, among other characteristics, reactor configuration, reactant concentration, surrounding gas environment composition, feed composition, imposed fluid thermal environment, etc., or any combination thereof.
[0149] 8 is a plot of a demonstration example of increasing reactor yield with increasing reactor pressure, according to one embodiment. The plot can represent a simulation generated using the CNATERA software framework.
[0150] While preferred embodiments of the present invention have been shown and described herein, it will be apparent to those skilled in the art that such embodiments are provided by way of example only. It is not intended that the present invention be limited by the specific examples provided in the specification. Although the present invention has been described in conjunction with the foregoing specification, the description and illustration of the embodiments herein are not intended to be construed in a limiting sense. Numerous variations, changes, and substitutions will occur to those skilled in the art at this point without departing from the present invention. Furthermore, it is to be understood that all aspects of the present invention are not limited to the specific depictions, configurations, or relative proportions set forth herein, which depend upon a variety of conditions and variables. It should be understood that various alternatives to the embodiments of the present invention described herein may be used in practicing the present invention. It is therefore contemplated that the present invention shall cover such alternatives, modifications, variations, or equivalents. It is intended that the following claims define the scope of the present invention, and that methods and structures within the scope of these claims and their equivalents are covered thereby.
Claims
1. 1. A method for producing carbon particles in a reactor, comprising: (a) generating a plasma in the reactor using one or more electrodes; (b) injecting hydrocarbons into said reactor through one or more injectors, thereby producing said carbon particles; Including, the reactor is operated at a pressure of 1.5 bar or more; 30% or more of the carbon particles have an equivalent sphere diameter of less than 2 micrometers (μm); method.
2. The method of claim 1 , wherein the one or more electrodes comprise an AC electrode or a DC electrode.
3. The method of claim 1 further comprising the step of producing hydrogen, wherein the hydrogen and the carbon particles are produced in a once-through, single-stage process.
4. The method of claim 1 , wherein the hydrocarbon is a gas that is heated upon contact with the plasma.
5. 10. The method of claim 1, wherein the carbon particles have 90% of the surface area compared to carbon particles formed in the reactor when operated at a pressure of 1 bar.
6. 10. The method of claim 1, wherein the reactor is operated at a pressure of 5 bar or greater, and the carbon particles have 60% of the surface area compared to carbon particles formed in the reactor when operated at a pressure of 1 bar.
7. 10. The method of claim 1, wherein the carbon particles have 35% of the surface area compared to carbon particles formed in the reactor when operated at a pressure of 1 bar.
8. The method of claim 1 , further comprising the step of including one or more additives in the carbon particles to increase the surface area of the carbon particles.
9. The method of claim 8 , wherein the one or more additives comprise a hydrocarbon gas.
10. The method of claim 8 , wherein the one or more additives include silicon.
11. The method of claim 8 , wherein the one or more additives comprises an aromatic additive.
12. 10. The method of claim 1, wherein the reactor comprises an oxygen-free environment of less than 2% molecular oxygen by volume or molar.
13. 4. The method of claim 3, further comprising isolating the carbon particles using a pressure lock system to remove at least a portion of the hydrogen produced and reducing the pressure of the atmosphere surrounding the carbon particles to less than 1.5 bar.
14. 4. The method of claim 3, wherein the hydrogen is produced at a rate greater than 0.5 tonnes per hour.
15. The method of claim 1 further comprising adding a sheath gas to the reactor.