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WO2025135042A1 - Procédé de production de carbone et d'hydrogène, et fibre de carbone - Google Patents

Procédé de production de carbone et d'hydrogène, et fibre de carbone Download PDF

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Publication number
WO2025135042A1
WO2025135042A1 PCT/JP2024/044652 JP2024044652W WO2025135042A1 WO 2025135042 A1 WO2025135042 A1 WO 2025135042A1 JP 2024044652 W JP2024044652 W JP 2024044652W WO 2025135042 A1 WO2025135042 A1 WO 2025135042A1
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Prior art keywords
carbon
reaction zone
hydrogen
catalyst
carbon fiber
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English (en)
Japanese (ja)
Inventor
直毅 横川
昌輝 小坂
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Sumitomo Chemical Co Ltd
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Sumitomo Chemical Co Ltd
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    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
    • B01J23/70—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper
    • B01J23/74—Iron group metals
    • B01J23/745—Iron
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
    • C01B3/02—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen
    • C01B3/22—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by decomposition of gaseous or liquid organic compounds
    • C01B3/24—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by decomposition of gaseous or liquid organic compounds of hydrocarbons
    • C01B3/26—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by decomposition of gaseous or liquid organic compounds of hydrocarbons using catalysts
    • D—TEXTILES; PAPER
    • D01—NATURAL OR MAN-MADE THREADS OR FIBRES; SPINNING
    • D01F—CHEMICAL FEATURES IN THE MANUFACTURE OF ARTIFICIAL FILAMENTS, THREADS, FIBRES, BRISTLES OR RIBBONS; APPARATUS SPECIALLY ADAPTED FOR THE MANUFACTURE OF CARBON FILAMENTS
    • D01F9/00—Artificial filaments or the like of other substances; Manufacture thereof; Apparatus specially adapted for the manufacture of carbon filaments
    • D01F9/08—Artificial filaments or the like of other substances; Manufacture thereof; Apparatus specially adapted for the manufacture of carbon filaments of inorganic material
    • D01F9/12—Carbon filaments; Apparatus specially adapted for the manufacture thereof
    • D01F9/127—Carbon filaments; Apparatus specially adapted for the manufacture thereof by thermal decomposition of hydrocarbon gases or vapours or other carbon-containing compounds in the form of gas or vapour, e.g. carbon monoxide, alcohols

Definitions

  • the present invention relates to a method for producing carbon and hydrogen, and to carbon fibers.
  • Patent Document 1 a process for obtaining hydrogen and carbon by pyrolysis of hydrocarbons has been known.
  • the present invention was made in consideration of the above problems, and aims to provide a method for producing carbon and hydrogen that can produce carbon with high bulk density, and a new carbon fiber obtained thereby.
  • [1] pyrolysis of hydrocarbons in a first reaction zone to produce carbon and hydrogen; and a step of thermally decomposing hydrocarbons in a second reaction zone having a higher temperature than the first reaction zone using the carbon as a catalyst in the presence of the carbon produced in the first reaction zone to obtain carbon and hydrogen, wherein a partial pressure of hydrocarbons in the first reaction zone is 0.02 MPa or more, and the carbon obtained in the second reaction zone has a bulk density of 0.3 g/cm3 or more and an aspect ratio of 2 or more.
  • [7] The method for producing carbon and hydrogen according to any one of [1] to [6], further comprising a heating device for heating at least one of the first reaction zone and the second reaction zone.
  • [8] The method for producing carbon and hydrogen according to any one of [1] to [7], wherein at least one of carbon and hydrocarbons produced in the first reaction zone and supplied to the second reaction zone is heated before being supplied to the second reaction zone.
  • [9] The method for producing carbon and hydrogen according to any one of [1] to [8], wherein the hydrocarbon is thermally decomposed in the presence of an oxide of a transition metal in the first reaction zone.
  • the present invention provides a method for producing carbon and hydrogen that can produce carbon with high bulk density, and a novel carbon fiber obtained thereby.
  • FIG. 1(a) is a low-magnification TEM image of carbon ⁇ produced in the first reaction zone in Example 1 and used as a catalyst in the second reaction zone
  • FIG. 1(b) is a high-magnification image of a different field of view of FIG. 1(a).
  • FIG. 2(a) is a low-magnification TEM image of Carbon A produced in the second reaction zone of Example 1
  • FIG. 2(b) is a high-magnification image of a different field of view from FIG. 2(a).
  • FIG. 3(a) is a low-magnification TEM image of carbon B produced in the second reaction zone of Example 2
  • FIG. 3(b) is a low-magnification image of a different field of view from FIG. 3(a).
  • the method for producing hydrogen and carbon includes the steps of: (1) pyrolyzing hydrocarbons in a first reaction zone to produce carbon and hydrogen; (2) pyrolyzing hydrocarbons in the presence of carbon produced in the first reaction zone in a second reaction zone having a higher temperature than the first reaction zone to obtain carbon and hydrogen.
  • Step In this step hydrocarbons are thermally cracked in a first reaction zone to produce carbon and hydrogen.
  • hydrocarbons there are no particular limitations on the hydrocarbons, and methane, ethane, etc. can be used, or a mixed gas can be used.
  • the hydrocarbons can be aliphatic or aromatic.
  • the temperature of the first reaction zone there are no particular limitations on the temperature of the first reaction zone, but from the perspective of producing carbon fibers with a large G/D ratio (e.g., a G/D ratio of 1 or more), such as carbon nanotubes, a temperature of 500 to 900°C is preferable.
  • a G/D ratio of 1 or more such as carbon nanotubes
  • the partial pressure of the hydrocarbons in the first reaction zone is preferably high from the viewpoint of producing carbon with high bulk density in the second reaction zone, and is preferably 0.02 MPa or more, may be 0.03 MPa or more, may be 0.05 MPa or more, or may be 0.08 MPa or more.
  • the pressure in the first reaction zone is not particularly limited, but is preferably 0.1 to 5 MPa.
  • the gas supplied to the first reaction zone may contain a gas other than a hydrocarbon.
  • the gas other than a hydrocarbon include an inert gas such as argon, nitrogen, hydrogen, CO, and CO2 .
  • the partial pressure of the gas other than a hydrocarbon is preferably lower than the partial pressure of the hydrocarbon, and may be 1/2 or less, 1/5 or less, or 1/10 or less of the partial pressure of the hydrocarbon.
  • the catalyst examples include transition metals and transition metal oxides.
  • transition metals are Fe, Ni, Co, Pd, and Pt.
  • the catalyst may be iron (III) oxide. From the viewpoint of increasing the amount of carbon produced in the first reaction zone and increasing the bulk density of the carbon produced in the second reaction zone, the catalyst is preferably an oxide of a transition metal, and in particular, iron (III) oxide.
  • the catalyst particles may be supported on a carrier.
  • the carrier may be porous. Examples of carriers are alpha-alumina and gamma-alumina.
  • the reaction vessel that forms the first reaction zone may be a fixed bed or a fluidized bed of the catalyst or its carrier.
  • the catalyst may be fed to the reaction vessel in batches, or the catalyst may be continuously discharged from the reaction vessel, regenerated, and then continuously fed to the reactor.
  • the heating means for the first reaction zone is not particularly limited, and can be, for example, an electric heater, an infrared heater, a heat transfer tube through which a heat medium such as combustion exhaust gas flows, a microwave heating device, or a gas and/or catalyst preheating device that heats the hydrocarbon gas and/or catalyst before supplying it to the reaction vessel.
  • the carbon obtained in the first reaction zone may be carbon fibers, such as carbon nanotubes.
  • the diameter of the carbon fibers may be between 5 and 200 nm.
  • the G/D ratio of the carbon fibers may be 1 or greater.
  • the carbon nanotubes may be single-wall nanotubes or multi-wall nanotubes.
  • Step 2 hydrocarbons are thermally decomposed in a second reaction zone having a higher temperature than the first reaction zone in the presence of carbon produced in the first reaction zone to obtain carbon and hydrogen.
  • the partial pressure of the hydrocarbon in the second reaction zone is preferably 0.02 MPa or more in order to produce carbon with high bulk density, and may be 0.03 MPa or more, 0.05 MPa or more, or 0.08 MPa or more.
  • the hydrocarbon supplied in the second reaction zone may be the same as or different from the hydrocarbon supplied in the first reaction zone.
  • the partial pressure of the hydrocarbon in the first reaction zone and the partial pressure of the hydrocarbon in the second reaction zone may be the same or different.
  • the temperature difference between the first and second reaction zones may be 100 to 500°C.
  • the temperature of the second reaction zone is preferably between 900°C and 1200°C.
  • the reaction vessel and heating method of the second reaction zone examples of which are as shown for the first reaction zone.
  • the pressure in the second reaction zone there is no particular limit to the pressure in the second reaction zone, but it is preferable to set it to 0.1 to 5 MPa.
  • the pressure in the first reaction zone and the pressure in the second reaction zone may be the same or different.
  • Gas containing hydrogen and hydrocarbons discharged from the first reaction zone may be supplied to the second reaction zone, or hydrocarbons supplied from a source other than the first reaction zone may be supplied to the second reaction zone, or these may be mixed and supplied to the second reaction zone.
  • the carbon produced in the first reaction zone When the carbon produced in the first reaction zone is supplied to the second reaction zone, the carbon produced may be supplied to the second reaction zone together with the catalyst, or the carbon produced may be supplied to the second reaction zone after removing at least a portion of the catalyst.
  • the heating means for the second reaction zone is not particularly limited, and may be, for example, an electric heater, an infrared heater, a heat transfer tube through which a heat medium such as combustion exhaust gas flows, or a microwave heating device.
  • the heating means may also be a preheating device that heats at least one of the hydrocarbon-containing gas, catalyst, and carbon discharged from the first reaction zone, or a preheating device that heats the hydrocarbons supplied to the second reaction zone separately from the first reaction zone.
  • the gas supplied to the second reaction zone may contain a gas other than a hydrocarbon.
  • the gas other than a hydrocarbon include an inert gas such as argon, nitrogen, hydrogen, CO, and CO2 .
  • the partial pressure of the gas other than a hydrocarbon is preferably lower than the partial pressure of the hydrocarbon, and may be 1/2 or less, 1/5 or less, or 1/10 or less of the partial pressure of the hydrocarbon.
  • the gas other than a hydrocarbon supplied to the second reaction zone may be the same as or different from the gas other than a hydrocarbon in the first reaction zone. From the viewpoint of hydrogen utilization, it is preferable that the partial pressure of the gas other than a hydrocarbon is low.
  • hydrocarbon supplied to the second reaction zone methane, ethane, or a mixture of these gases can be used, and the hydrocarbon may be the same as or different from the hydrocarbon supplied to the first reaction zone.
  • the hydrogen produced by this method can be separated from hydrocarbons and other substances and then used in a variety of ways, including for power generation.
  • This process produces carbon fibers with high bulk density.
  • the temperature is increased only in the first reaction zone without carrying out the two-stage reaction, carbon fibers having a low G/D ratio (eg, less than 1) tend to be produced, making it difficult to produce carbon fibers having a high bulk density.
  • the high partial pressure of the hydrocarbons in the gas supplied makes it easier to obtain carbon with a bulk density of 0.3 g/cm 3 or more in the second reaction zone. The reason for this is also unclear, but it may be that the high partial pressure of the hydrocarbons supplied to the first reaction zone contributes to the dense structure of the carbon produced in the first reaction zone.
  • Carbon fiber (Carbon fiber)
  • the carbon fibers obtained by the above-mentioned method have a bulk density of 0.1 g/cm 3 or more, an aspect ratio of 2 or more, and a diameter of less than 1000 nm.
  • the bulk density of the carbon fiber may be 0.2 g/ cm3 or more, or 0.3 g/ cm3 or more.
  • the bulk density may be 1.0 g/ cm3 or less.
  • the aspect ratio of the carbon fibers can typically be 5 or more, and can be 10 or more.
  • the diameter of the carbon fiber is less than 1000 nm, and may be 500 nm or less, 300 nm or less, or 200 nm or less.
  • the diameter of the carbon fiber may be 10 nm or more, or 20 nm or more.
  • the diameter and aspect ratio may be the average of measurements at 10 points on the TEM photograph.
  • the G/D ratio may be 1 or less, 0.9 or less, 0.8 or less, or 0.7 or less. This condition indicates that the carbon fiber has many parts that do not exhibit a graphite structure.
  • the exothermic peak that appears at 500°C or higher appears at 650°C or higher, and preferably 700°C or higher. This means that the carbon fiber is less susceptible to oxidation than normal, and has the advantage of being easier to store and transport.
  • the carbon fiber has a specific surface area measured by the BET method of 4 m 2 /g or more.
  • Such carbon fibers have a high bulk density, making them easy to handle and easy to add to resins, and can be used as a thermal conductivity enhancer. They can also be used as a conductive additive in battery electrodes. They can also be mixed into asphalt pavement.
  • Example 1 (Catalyst A ⁇ Carbon ⁇ ⁇ Carbon A)
  • the iron-supported alumina catalyst used in Example 1 was synthesized by the following procedure.
  • a gamma-alumina carrier manufactured by Sumitomo Chemical Co., Ltd. (alumina content 96 wt %, silica content 4 wt %) was crushed in a mortar, and the crushed alumina was classified using metal sieves with 45 ⁇ m and 90 ⁇ m openings to obtain a carrier with a particle size range of 45 to 90 ⁇ m.
  • a TEM photograph of the carbon ⁇ obtained in the first reaction zone is shown in Figure 1. It was confirmed that the carbon ⁇ obtained in the first reaction zone has a carbon nanotube structure.
  • the second reaction zone was the same as the first reaction zone, and 0.1 g of the carbon ⁇ obtained above was dispersed and introduced into a sample dish. While flowing methane at a rate of 15 mL/min, the temperature was raised to 1000°C from the outside using an electric furnace, and after the internal temperature reached 1000°C, it was held for 3 hours. After the reaction, the solid matter on the sample dish in the reactor was collected to obtain 0.37 g of carbon A. The ratio of the weight increase of the sample dish (carbon A) to the weight of carbon ⁇ as a catalyst was 3.7. Almost no soot stains were observed on the inner wall of the reaction tube, and the amount was below the detection limit. The weight increase in the two stages (carbon ⁇ + carbon A) and the catalyst A charging ratio were 54.4.
  • the carbon ⁇ obtained in the first reaction zone and the carbon A obtained in the second reaction zone were analyzed for bulk density, thermal analysis by TG-DTA, BET specific surface area, graphite/diamond ratio by microscopic laser Raman analysis, amount of contained elements, etc.
  • the measurement results are summarized in Tables 1 and 2.
  • a TEM photograph is shown in Figure 2.
  • the aspect ratio of carbon A was 2 or more.
  • TG-DTA thermal analysis Measurement was carried out under the following conditions using a differential thermal-thermogravimetric simultaneous measurement device Thermo plus Evo2 TG-DTA8122 manufactured by Rigaku Corporation.
  • Sample pan Platinum Reference sample: Alumina standard sample Measurement conditions: Heating from room temperature to 1000° C. at a heating rate of 10° C./min Measurement atmosphere: Air flow at 500 mL/min Exothermic peak temperature: The temperature at which the heat absorption in differential thermal analysis was maximum was used.
  • BET specific surface area Measured using BELSORP-mini manufactured by BEL Japan Co., Ltd. under the following treatment conditions.
  • Pretreatment device BELPREP-vac2 manufactured by Japan BEL Co., Ltd.
  • Pretreatment conditions 120° C. for 2 hours, vacuum degassing
  • Nitrogen adsorption/desorption isotherm was measured using a constant volume method.
  • Adsorbate Nitrogen Saturation vapor pressure: Measured adsorbate cross-sectional area: 0.162 nm Sample amount: 50 mg
  • Graphite/Diamond Ratio The G/D ratio was measured by subjecting carbon to microscopic laser Raman spectroscopy under the following conditions using a Nanophoton RAMAN-11. The G/D ratio was calculated as the peak intensity ratio by measuring the maximum peak intensity in each of the following bands.
  • Graphite band 1578 cm -1 to 1590 cm -1
  • Diamond-band 1339 cm -1 to 1357 cm -1
  • Measurement location Surface excitation wavelength: 532 nm Grating: 600 grooves/mm
  • Objective lens ⁇ 20, N.A. 0.45 Wave number range: 110 cm -1 to 2000 cm -1
  • the amounts of elements contained in carbon ⁇ and carbon A were calculated as follows.
  • the Fe atom content in catalyst A was 50 wt%
  • the Al atom content was 26 wt%
  • the other components were 24 wt%.
  • the amounts of elements contained in the generated carbon ⁇ and carbon A were calculated from the total weight of the generated carbon and the initial weight of the catalyst, assuming that the catalyst was uniformly dispersed in the generated carbon material.
  • the contents of elements contained in carbon ⁇ and carbon A can also be measured by elemental analysis methods such as high-frequency inductively coupled plasma optical emission spectrometry or X-ray fluorescence analysis.
  • Example 2 (Catalyst A ⁇ Carbon ⁇ ⁇ Carbon B) Carbon B was synthesized using carbon ⁇ as a catalyst in the same manner as in Example 1, except that the reaction time in the second reaction zone was changed to 6 hours.
  • the ratio of the weight increase (carbon B) of the catalyst boat after holding to the amount of carbon ⁇ charged as a catalyst was 6.6. Almost no soot fouling was observed on the inner wall of the reaction tube, and the amount was below the detection limit.
  • the ratio of the weight increase (carbon ⁇ + carbon B) in the two stages to the catalyst A charge was 97.0.
  • the obtained carbon B was analyzed for bulk density, thermal analysis by TG-DTA, and BET specific surface area, and the bulk density and the amount of graphite and diamond-specific elements were analyzed by microscopic laser Raman analysis.
  • the measurement results are summarized in Tables 1 and 2.
  • a TEM photograph is shown in Figure 3.
  • the aspect ratio of carbon B was 2 or more.
  • the carbon material obtained in this application has a higher bulk density than commercially available carbon nanotubes, yet has a higher thermal decomposition temperature.
  • Comparative Example 2 (Catalyst A ⁇ Carbon ⁇ ⁇ Carbon C) (Production of Carbon ⁇ with Catalyst A in the First Reaction Zone)
  • 0.05 g of catalyst A was dispersed in a quartz sample dish of 2.0 cm x 7.7 cm and introduced into a quartz tube having a diameter of 36.0 cm.
  • Methane was circulated at a rate of 15 mL/min and nitrogen was circulated at a rate of 285 mL/min (i.e., methane partial pressure was 0.005 MPa), and the temperature was raised to 700°C from the outside using an electric furnace. After the internal temperature reached 700°C, the temperature was maintained for 6 hours.
  • the solid matter (carbon ⁇ ) on the sample dish in the reactor was collected and its weight was measured.
  • the weight increase obtained by subtracting the weight of the catalyst from the weight of the collected solid matter was calculated as the produced carbon, and the weight ratio of the catalyst A introduced was calculated to be 1.1 (carbon ⁇ -g/catalyst A-g).
  • the second reaction zone was the same as the first reaction zone, and 0.1 g of the carbon ⁇ obtained above was dispersed and introduced into a sample dish. While flowing methane at a rate of 15 mL/min, the temperature was raised to 1000°C from the outside using an electric furnace, and after the internal temperature reached 1000°C, it was held for 3 hours.

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  • Engineering & Computer Science (AREA)
  • Organic Chemistry (AREA)
  • General Health & Medical Sciences (AREA)
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  • Combustion & Propulsion (AREA)
  • Inorganic Chemistry (AREA)
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Abstract

L'invention concerne un procédé de production de carbone et d'hydrogène, le procédé comprenant : une étape de décomposition thermique d'un hydrocarbure dans une première zone de réaction pour générer du carbone et de l'hydrogène ; et une étape de décomposition thermique d'un hydrocarbure dans une seconde zone de réaction en présence du carbone généré dans la première zone de réaction en utilisant le carbone en tant que catalyseur pour obtenir du carbone et de l'hydrogène, la seconde zone de réaction ayant une température supérieure à celle de la première zone de réaction. Dans le procédé, la pression partielle de l'hydrocarbure dans la première zone de réaction est de 0,02 MPa ou plus, et le carbone obtenu dans la seconde zone de réaction a une densité apparente de 0,3 g/cm3 ou plus et un rapport d'aspect de 2 ou plus.
PCT/JP2024/044652 2023-12-22 2024-12-17 Procédé de production de carbone et d'hydrogène, et fibre de carbone Pending WO2025135042A1 (fr)

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JP2023217324 2023-12-22
JP2023-217324 2023-12-22

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Citations (10)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPS61119714A (ja) * 1984-11-13 1986-06-06 Asahi Chem Ind Co Ltd 炭素繊維の製造法
JPH08165101A (ja) * 1994-12-14 1996-06-25 Agency Of Ind Science & Technol 水素の製造方法
JP2006183225A (ja) * 2004-08-31 2006-07-13 Bussan Nanotech Research Institute Inc 炭素繊維構造体
JP2013502361A (ja) * 2009-08-21 2013-01-24 バイエル・マテリアルサイエンス・アクチェンゲゼルシャフト カーボンナノチューブ凝集体
WO2013099256A1 (fr) * 2011-12-27 2013-07-04 昭和電工株式会社 Procédé de production de fibres de carbone
JP2013189605A (ja) * 2012-03-15 2013-09-26 Toshiba Corp 熱輸送流体
JP2016520510A (ja) * 2013-06-07 2016-07-14 コベストロ・ドイチュラント・アクチェンゲゼルシャフト 多層カーボンナノチューブの製造方法、多層カーボンナノチューブおよびカーボンナノチューブ粉末
JP2021031382A (ja) * 2019-08-14 2021-03-01 ゼネラル・エレクトリック・カンパニイ 水素ガスおよび炭素生成物を生成するための生産システムおよび方法
US20210395090A1 (en) * 2017-04-21 2021-12-23 Shandong Dazhan Nano Materials Co., Ltd. Device and method for single-stage continuous preparation of carbon nanotubes
JP2023009119A (ja) * 2017-03-31 2023-01-19 ハイドロ－ケベック 粗カーボンナノチューブの精製のための方法

Patent Citations (10)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPS61119714A (ja) * 1984-11-13 1986-06-06 Asahi Chem Ind Co Ltd 炭素繊維の製造法
JPH08165101A (ja) * 1994-12-14 1996-06-25 Agency Of Ind Science & Technol 水素の製造方法
JP2006183225A (ja) * 2004-08-31 2006-07-13 Bussan Nanotech Research Institute Inc 炭素繊維構造体
JP2013502361A (ja) * 2009-08-21 2013-01-24 バイエル・マテリアルサイエンス・アクチェンゲゼルシャフト カーボンナノチューブ凝集体
WO2013099256A1 (fr) * 2011-12-27 2013-07-04 昭和電工株式会社 Procédé de production de fibres de carbone
JP2013189605A (ja) * 2012-03-15 2013-09-26 Toshiba Corp 熱輸送流体
JP2016520510A (ja) * 2013-06-07 2016-07-14 コベストロ・ドイチュラント・アクチェンゲゼルシャフト 多層カーボンナノチューブの製造方法、多層カーボンナノチューブおよびカーボンナノチューブ粉末
JP2023009119A (ja) * 2017-03-31 2023-01-19 ハイドロ－ケベック 粗カーボンナノチューブの精製のための方法
US20210395090A1 (en) * 2017-04-21 2021-12-23 Shandong Dazhan Nano Materials Co., Ltd. Device and method for single-stage continuous preparation of carbon nanotubes
JP2021031382A (ja) * 2019-08-14 2021-03-01 ゼネラル・エレクトリック・カンパニイ 水素ガスおよび炭素生成物を生成するための生産システムおよび方法

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