JP7329534B2 - 溶融塩ベースの触媒系を用いた高温熱分解 - Google Patents
溶融塩ベースの触媒系を用いた高温熱分解 Download PDFInfo
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- JP7329534B2 JP7329534B2 JP2020555204A JP2020555204A JP7329534B2 JP 7329534 B2 JP7329534 B2 JP 7329534B2 JP 2020555204 A JP2020555204 A JP 2020555204A JP 2020555204 A JP2020555204 A JP 2020555204A JP 7329534 B2 JP7329534 B2 JP 7329534B2
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- molten salt
- chloride
- methane
- hydrogen
- catalyst system
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- 150000003839 salts Chemical class 0.000 title claims description 33
- 239000003054 catalyst Substances 0.000 title claims description 30
- 238000000197 pyrolysis Methods 0.000 title description 11
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 claims description 74
- 238000006243 chemical reaction Methods 0.000 claims description 42
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 38
- 229910052799 carbon Inorganic materials 0.000 claims description 32
- 229910052751 metal Inorganic materials 0.000 claims description 32
- 239000002184 metal Substances 0.000 claims description 32
- 239000001257 hydrogen Substances 0.000 claims description 25
- 229910052739 hydrogen Inorganic materials 0.000 claims description 25
- 238000000034 method Methods 0.000 claims description 22
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 claims description 19
- 239000007787 solid Substances 0.000 claims description 19
- XEEYBQQBJWHFJM-UHFFFAOYSA-N iron Substances [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 claims description 17
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 claims description 14
- 239000007789 gas Substances 0.000 claims description 12
- 150000002739 metals Chemical class 0.000 claims description 11
- 229910052742 iron Inorganic materials 0.000 claims description 10
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 claims description 9
- 229910052802 copper Inorganic materials 0.000 claims description 9
- 239000010949 copper Substances 0.000 claims description 9
- 239000002245 particle Substances 0.000 claims description 9
- 239000000203 mixture Substances 0.000 claims description 8
- 229910017052 cobalt Inorganic materials 0.000 claims description 7
- 239000010941 cobalt Substances 0.000 claims description 7
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 claims description 7
- 229910052759 nickel Inorganic materials 0.000 claims description 7
- HCHKCACWOHOZIP-UHFFFAOYSA-N Zinc Chemical compound [Zn] HCHKCACWOHOZIP-UHFFFAOYSA-N 0.000 claims description 6
- WPBNNNQJVZRUHP-UHFFFAOYSA-L manganese(2+);methyl n-[[2-(methoxycarbonylcarbamothioylamino)phenyl]carbamothioyl]carbamate;n-[2-(sulfidocarbothioylamino)ethyl]carbamodithioate Chemical compound [Mn+2].[S-]C(=S)NCCNC([S-])=S.COC(=O)NC(=S)NC1=CC=CC=C1NC(=S)NC(=O)OC WPBNNNQJVZRUHP-UHFFFAOYSA-L 0.000 claims description 6
- 229910052725 zinc Inorganic materials 0.000 claims description 6
- 239000011701 zinc Substances 0.000 claims description 6
- TWRXJAOTZQYOKJ-UHFFFAOYSA-L Magnesium chloride Chemical compound [Mg+2].[Cl-].[Cl-] TWRXJAOTZQYOKJ-UHFFFAOYSA-L 0.000 claims description 4
- ZOKXTWBITQBERF-UHFFFAOYSA-N Molybdenum Chemical compound [Mo] ZOKXTWBITQBERF-UHFFFAOYSA-N 0.000 claims description 4
- WCUXLLCKKVVCTQ-UHFFFAOYSA-M Potassium chloride Chemical compound [Cl-].[K+] WCUXLLCKKVVCTQ-UHFFFAOYSA-M 0.000 claims description 4
- FAPWRFPIFSIZLT-UHFFFAOYSA-M Sodium chloride Chemical compound [Na+].[Cl-] FAPWRFPIFSIZLT-UHFFFAOYSA-M 0.000 claims description 4
- KWGKDLIKAYFUFQ-UHFFFAOYSA-M lithium chloride Chemical compound [Li+].[Cl-] KWGKDLIKAYFUFQ-UHFFFAOYSA-M 0.000 claims description 4
- 239000000155 melt Substances 0.000 claims description 4
- 229910052750 molybdenum Inorganic materials 0.000 claims description 4
- 239000011733 molybdenum Substances 0.000 claims description 4
- ATJFFYVFTNAWJD-UHFFFAOYSA-N Tin Chemical compound [Sn] ATJFFYVFTNAWJD-UHFFFAOYSA-N 0.000 claims description 3
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 claims description 3
- 229910001615 alkaline earth metal halide Inorganic materials 0.000 claims description 3
- 229910052793 cadmium Inorganic materials 0.000 claims description 3
- BDOSMKKIYDKNTQ-UHFFFAOYSA-N cadmium atom Chemical compound [Cd] BDOSMKKIYDKNTQ-UHFFFAOYSA-N 0.000 claims description 3
- -1 iron halides Chemical class 0.000 claims description 3
- 230000008018 melting Effects 0.000 claims description 3
- 238000002844 melting Methods 0.000 claims description 3
- 229910052718 tin Inorganic materials 0.000 claims description 3
- 239000010936 titanium Substances 0.000 claims description 3
- 229910052719 titanium Inorganic materials 0.000 claims description 3
- UXVMQQNJUSDDNG-UHFFFAOYSA-L Calcium chloride Chemical compound [Cl-].[Cl-].[Ca+2] UXVMQQNJUSDDNG-UHFFFAOYSA-L 0.000 claims description 2
- WDIHJSXYQDMJHN-UHFFFAOYSA-L barium chloride Chemical compound [Cl-].[Cl-].[Ba+2] WDIHJSXYQDMJHN-UHFFFAOYSA-L 0.000 claims description 2
- 229910001626 barium chloride Inorganic materials 0.000 claims description 2
- AIYUHDOJVYHVIT-UHFFFAOYSA-M caesium chloride Chemical compound [Cl-].[Cs+] AIYUHDOJVYHVIT-UHFFFAOYSA-M 0.000 claims description 2
- 239000001110 calcium chloride Substances 0.000 claims description 2
- 229910001628 calcium chloride Inorganic materials 0.000 claims description 2
- 229910001629 magnesium chloride Inorganic materials 0.000 claims description 2
- 239000001103 potassium chloride Substances 0.000 claims description 2
- 235000011164 potassium chloride Nutrition 0.000 claims description 2
- 239000011780 sodium chloride Substances 0.000 claims description 2
- 229910001631 strontium chloride Inorganic materials 0.000 claims description 2
- AHBGXTDRMVNFER-UHFFFAOYSA-L strontium dichloride Chemical compound [Cl-].[Cl-].[Sr+2] AHBGXTDRMVNFER-UHFFFAOYSA-L 0.000 claims description 2
- 239000000047 product Substances 0.000 description 15
- 238000000926 separation method Methods 0.000 description 7
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 description 6
- 150000002431 hydrogen Chemical class 0.000 description 6
- 229910044991 metal oxide Inorganic materials 0.000 description 6
- 150000004706 metal oxides Chemical class 0.000 description 6
- 238000000354 decomposition reaction Methods 0.000 description 5
- 150000001247 metal acetylides Chemical class 0.000 description 5
- 230000015572 biosynthetic process Effects 0.000 description 4
- 230000003197 catalytic effect Effects 0.000 description 4
- 229910002092 carbon dioxide Inorganic materials 0.000 description 3
- 229910021386 carbon form Inorganic materials 0.000 description 3
- 238000005229 chemical vapour deposition Methods 0.000 description 3
- 239000000446 fuel Substances 0.000 description 3
- 239000011833 salt mixture Substances 0.000 description 3
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 description 2
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 2
- 229910001508 alkali metal halide Inorganic materials 0.000 description 2
- 150000008045 alkali metal halides Chemical class 0.000 description 2
- 239000001569 carbon dioxide Substances 0.000 description 2
- 239000003575 carbonaceous material Substances 0.000 description 2
- 150000001875 compounds Chemical class 0.000 description 2
- 238000000151 deposition Methods 0.000 description 2
- 230000008021 deposition Effects 0.000 description 2
- 238000009826 distribution Methods 0.000 description 2
- 238000000227 grinding Methods 0.000 description 2
- 229930195733 hydrocarbon Natural products 0.000 description 2
- 150000002430 hydrocarbons Chemical class 0.000 description 2
- 238000004519 manufacturing process Methods 0.000 description 2
- 239000000463 material Substances 0.000 description 2
- 238000003786 synthesis reaction Methods 0.000 description 2
- 229920000049 Carbon (fiber) Polymers 0.000 description 1
- 239000004215 Carbon black (E152) Substances 0.000 description 1
- 230000002411 adverse Effects 0.000 description 1
- 239000003513 alkali Substances 0.000 description 1
- 229910021529 ammonia Inorganic materials 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 150000001721 carbon Chemical class 0.000 description 1
- 239000004917 carbon fiber Substances 0.000 description 1
- 239000002041 carbon nanotube Substances 0.000 description 1
- 229910021393 carbon nanotube Inorganic materials 0.000 description 1
- 238000000975 co-precipitation Methods 0.000 description 1
- 239000013065 commercial product Substances 0.000 description 1
- 238000005260 corrosion Methods 0.000 description 1
- 230000007797 corrosion Effects 0.000 description 1
- 238000005262 decarbonization Methods 0.000 description 1
- 239000006185 dispersion Substances 0.000 description 1
- 238000011143 downstream manufacturing Methods 0.000 description 1
- 239000000835 fiber Substances 0.000 description 1
- 239000011888 foil Substances 0.000 description 1
- 239000002803 fossil fuel Substances 0.000 description 1
- 150000004820 halides Chemical class 0.000 description 1
- 238000003621 hammer milling Methods 0.000 description 1
- 238000010438 heat treatment Methods 0.000 description 1
- 238000001027 hydrothermal synthesis Methods 0.000 description 1
- 239000011261 inert gas Substances 0.000 description 1
- 229910001338 liquidmetal Inorganic materials 0.000 description 1
- 150000002736 metal compounds Chemical class 0.000 description 1
- 239000002923 metal particle Substances 0.000 description 1
- 239000006262 metallic foam Substances 0.000 description 1
- 230000000116 mitigating effect Effects 0.000 description 1
- 229910052757 nitrogen Inorganic materials 0.000 description 1
- 230000006911 nucleation Effects 0.000 description 1
- 238000010899 nucleation Methods 0.000 description 1
- 239000000049 pigment Substances 0.000 description 1
- 239000000843 powder Substances 0.000 description 1
- 239000002243 precursor Substances 0.000 description 1
- 239000002994 raw material Substances 0.000 description 1
- 230000008929 regeneration Effects 0.000 description 1
- 238000011069 regeneration method Methods 0.000 description 1
- 238000001179 sorption measurement Methods 0.000 description 1
- 238000001991 steam methane reforming Methods 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 238000005979 thermal decomposition reaction Methods 0.000 description 1
- 238000010792 warming Methods 0.000 description 1
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- C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
- C01B2203/12—Feeding the process for making hydrogen or synthesis gas
- C01B2203/1205—Composition of the feed
- C01B2203/1211—Organic compounds or organic mixtures used in the process for making hydrogen or synthesis gas
- C01B2203/1235—Hydrocarbons
- C01B2203/1241—Natural gas or methane
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
- C01B2203/16—Controlling the process
- C01B2203/1614—Controlling the temperature
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- Inorganic Chemistry (AREA)
- General Health & Medical Sciences (AREA)
- Combustion & Propulsion (AREA)
- Health & Medical Sciences (AREA)
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Description
本出願は、2018年4月9日出願の米国仮特許出願第62/654,587号の優先権を主張するものであり、その開示全体が参照により本明細書に組み込まれる。
本明細書は以下の発明の態様を包含する。
[項目1] アルカリ金属のハロゲン化物;アルカリ土類金属のハロゲン化物;亜鉛、銅、マンガン、カドミウム、スズおよび鉄のハロゲン化物;ならびにそれらの混合物からなる群から選択される溶融塩を含み、前記溶融塩が、その中に、微粉化された元素金属、金属酸化物、金属炭化物、またはそれらの混合物の形で、鉄、モリブデン、マンガン、ニッケル、コバルト、亜鉛、チタンおよび銅のうちの1つ以上の触媒活性形態を分散させている、700℃を超える反応温度でメタンを熱分解することに活性がある触媒系。
[項目2] 前記溶融塩が1000℃未満で溶融する、項目1に記載の触媒系。
[項目3] 前記溶融塩が約600℃~約800℃で溶融する、項目1または2に記載の触媒系。
[項目4] 前記分散された触媒活性金属を含有する粒子の平均サイズが約0.5mm以下である、項目1~3のいずれかに記載の触媒系。
[項目5] 前記溶融塩中に分散された触媒活性金属の濃度が、全触媒系の0.1~約20重量%の範囲である、項目1~4のいずれかに記載の触媒系。
[項目6] 反応条件下で項目1~5のいずれかに記載の触媒系を含む反応ゾーンにメタンを通過させて、水素を含むガス流および固体炭素生成物を生成することを含む、プロセス。
[項目7] 前記反応条件が700~1300℃の範囲の温度を含む、項目6に記載のプロセス。
Claims (6)
- 水素を含むガス流および固体炭素生成物を生成するプロセスであって、反応条件下で触媒系を含む反応ゾーンにメタンを通過させて、水素を含むガス流および固体炭素生成物を生成することを含み、
反応が600~1300℃の範囲の温度で実施され、
触媒系が、アルカリ金属のハロゲン化物;アルカリ土類金属のハロゲン化物;亜鉛、銅、マンガン、カドミウム、スズおよび鉄のハロゲン化物;ならびにそれらの混合物からなる群から選択される、1000℃未満で溶融する溶融塩を含み、前記溶融塩が、その中に元素金属、金属酸化物、金属炭化物、またはそれらの混合物として微細分散された粒子の形で、鉄、モリブデン、マンガン、ニッケル、コバルト、チタンおよび銅のうちの1つ以上の触媒活性形態を分散させており、前記微細分散された粒子の平均サイズが0.5mm以下である、プロセス。 - 前記反応条件が700~1300℃の範囲の温度を含む、請求項1に記載のプロセス。
- 前記溶融塩が600℃~800℃で溶融する、請求項1または2に記載のプロセス。
- 前記溶融塩中に分散された触媒活性金属の濃度が、全触媒系の0.1~20重量%の範囲である、請求項1~3のいずれかに記載のプロセス。
- 溶融塩が塩化リチウム、塩化ナトリウム、塩化カリウム、塩化セシウム、塩化マグネシウム、塩化カルシウム、塩化ストロンチウム、塩化バリウムまたはそれらの混合物を含む、請求項1~4のいずれかに記載のプロセス。
- 溶融塩に分散させた1つ以上の触媒活性形態が、鉄、コバルト、ニッケル及び銅のうちの1つ以上の触媒活性形態である、請求項1~5のいずれかに記載のプロセス。
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US201862654587P | 2018-04-09 | 2018-04-09 | |
US62/654,587 | 2018-04-09 | ||
PCT/EP2019/058453 WO2019197256A1 (en) | 2018-04-09 | 2019-04-04 | Pyrolysis of methane with a molten salt based catalyst system |
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AU (1) | AU2019252154B2 (ja) |
BR (1) | BR112020020508A2 (ja) |
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MX2023008009A (es) * | 2021-01-07 | 2023-09-25 | Univ Johns Hopkins | Produccion de hidrogeno a partir de hidrocarburos. |
EP4029924A1 (en) * | 2021-08-17 | 2022-07-20 | Shell Internationale Research Maatschappij B.V. | Pyrolytic process for thermal energy to chemical process |
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US3979332A (en) * | 1975-02-03 | 1976-09-07 | Shell Oil Company | High temperature methanation with molten salt-based catalyst systems |
US4665261A (en) * | 1985-06-21 | 1987-05-12 | Atlantic Richfield Company | Hydrocarbon conversion process using a molten salt |
US5767165A (en) * | 1995-03-16 | 1998-06-16 | Steinberg; Meyer | Method for converting natural gas and carbon dioxide to methanol and reducing CO2 emissions |
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EA038556B1 (ru) | 2021-09-14 |
EP3774644A1 (en) | 2021-02-17 |
JP2021520987A (ja) | 2021-08-26 |
CA3096297A1 (en) | 2019-10-17 |
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