JP2009544464A - 低温変換用の触媒及び一酸化炭素と水とを二酸化炭素と水素に低温で変換するための方法 - Google Patents
低温変換用の触媒及び一酸化炭素と水とを二酸化炭素と水素に低温で変換するための方法 Download PDFInfo
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- JP2009544464A JP2009544464A JP2009521229A JP2009521229A JP2009544464A JP 2009544464 A JP2009544464 A JP 2009544464A JP 2009521229 A JP2009521229 A JP 2009521229A JP 2009521229 A JP2009521229 A JP 2009521229A JP 2009544464 A JP2009544464 A JP 2009544464A
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- catalyst
- oxide
- mass
- hydrogen
- copper
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- 239000003054 catalyst Substances 0.000 title claims abstract description 148
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 title claims abstract description 46
- 229910002091 carbon monoxide Inorganic materials 0.000 title claims abstract description 46
- 229910052739 hydrogen Inorganic materials 0.000 title claims abstract description 43
- 239000001257 hydrogen Substances 0.000 title claims abstract description 38
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 title claims abstract description 37
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 title claims abstract description 28
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 title claims abstract description 22
- 229910002092 carbon dioxide Inorganic materials 0.000 title claims abstract description 11
- 239000001569 carbon dioxide Substances 0.000 title claims abstract description 10
- VUZPPFZMUPKLLV-UHFFFAOYSA-N methane;hydrate Chemical compound C.O VUZPPFZMUPKLLV-UHFFFAOYSA-N 0.000 title claims abstract description 10
- 238000000034 method Methods 0.000 title claims description 44
- 238000006243 chemical reaction Methods 0.000 title claims description 33
- 230000008569 process Effects 0.000 title claims description 11
- XLOMVQKBTHCTTD-UHFFFAOYSA-N Zinc monoxide Chemical compound [Zn]=O XLOMVQKBTHCTTD-UHFFFAOYSA-N 0.000 claims abstract description 45
- QPLDLSVMHZLSFG-UHFFFAOYSA-N Copper oxide Chemical compound [Cu]=O QPLDLSVMHZLSFG-UHFFFAOYSA-N 0.000 claims abstract description 37
- 239000011787 zinc oxide Substances 0.000 claims abstract description 23
- GDVKFRBCXAPAQJ-UHFFFAOYSA-A dialuminum;hexamagnesium;carbonate;hexadecahydroxide Chemical compound [OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[Mg+2].[Mg+2].[Mg+2].[Mg+2].[Mg+2].[Mg+2].[Al+3].[Al+3].[O-]C([O-])=O GDVKFRBCXAPAQJ-UHFFFAOYSA-A 0.000 claims abstract description 15
- 239000005751 Copper oxide Substances 0.000 claims abstract description 14
- 229910000431 copper oxide Inorganic materials 0.000 claims abstract description 14
- 229910001701 hydrotalcite Inorganic materials 0.000 claims abstract description 12
- 229960001545 hydrotalcite Drugs 0.000 claims abstract description 12
- 239000012018 catalyst precursor Substances 0.000 claims abstract description 9
- TWNQGVIAIRXVLR-UHFFFAOYSA-N oxo(oxoalumanyloxy)alumane Chemical compound O=[Al]O[Al]=O TWNQGVIAIRXVLR-UHFFFAOYSA-N 0.000 claims abstract description 9
- 239000000203 mixture Substances 0.000 claims description 35
- 239000010949 copper Substances 0.000 claims description 27
- 239000000446 fuel Substances 0.000 claims description 26
- 239000000463 material Substances 0.000 claims description 16
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 claims description 15
- 229910052802 copper Inorganic materials 0.000 claims description 15
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 claims description 14
- CDBYLPFSWZWCQE-UHFFFAOYSA-L Sodium Carbonate Chemical compound [Na+].[Na+].[O-]C([O-])=O CDBYLPFSWZWCQE-UHFFFAOYSA-L 0.000 claims description 10
- 238000004519 manufacturing process Methods 0.000 claims description 9
- 238000001556 precipitation Methods 0.000 claims description 7
- 239000002243 precursor Substances 0.000 claims description 7
- 239000011701 zinc Substances 0.000 claims description 7
- 229910052782 aluminium Inorganic materials 0.000 claims description 5
- 229910000029 sodium carbonate Inorganic materials 0.000 claims description 5
- 229910052725 zinc Inorganic materials 0.000 claims description 5
- HCHKCACWOHOZIP-UHFFFAOYSA-N Zinc Chemical compound [Zn] HCHKCACWOHOZIP-UHFFFAOYSA-N 0.000 claims description 4
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 claims description 4
- 229910000510 noble metal Inorganic materials 0.000 claims description 4
- 150000001875 compounds Chemical class 0.000 claims description 3
- RVTZCBVAJQQJTK-UHFFFAOYSA-N oxygen(2-);zirconium(4+) Chemical compound [O-2].[O-2].[Zr+4] RVTZCBVAJQQJTK-UHFFFAOYSA-N 0.000 claims description 3
- 229910001928 zirconium oxide Inorganic materials 0.000 claims description 3
- 239000007789 gas Substances 0.000 description 23
- 239000000243 solution Substances 0.000 description 21
- 229910018072 Al 2 O 3 Inorganic materials 0.000 description 19
- 230000015572 biosynthetic process Effects 0.000 description 13
- 238000003786 synthesis reaction Methods 0.000 description 13
- 229910052760 oxygen Inorganic materials 0.000 description 12
- 229910002651 NO3 Inorganic materials 0.000 description 10
- NHNBFGGVMKEFGY-UHFFFAOYSA-N Nitrate Chemical compound [O-][N+]([O-])=O NHNBFGGVMKEFGY-UHFFFAOYSA-N 0.000 description 10
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 9
- 239000001301 oxygen Substances 0.000 description 9
- 230000000694 effects Effects 0.000 description 8
- 238000012360 testing method Methods 0.000 description 8
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- 239000011651 chromium Substances 0.000 description 7
- 238000009833 condensation Methods 0.000 description 7
- 230000005494 condensation Effects 0.000 description 7
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 description 6
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 5
- 239000012159 carrier gas Substances 0.000 description 5
- 230000000052 comparative effect Effects 0.000 description 5
- 229930195733 hydrocarbon Natural products 0.000 description 5
- 150000002430 hydrocarbons Chemical class 0.000 description 5
- 150000002431 hydrogen Chemical class 0.000 description 5
- XEEYBQQBJWHFJM-UHFFFAOYSA-N iron Substances [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 5
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 5
- MWUXSHHQAYIFBG-UHFFFAOYSA-N Nitric oxide Chemical compound O=[N] MWUXSHHQAYIFBG-UHFFFAOYSA-N 0.000 description 4
- HSJPMRKMPBAUAU-UHFFFAOYSA-N cerium(3+);trinitrate Chemical compound [Ce+3].[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O HSJPMRKMPBAUAU-UHFFFAOYSA-N 0.000 description 4
- 238000005259 measurement Methods 0.000 description 4
- 230000002269 spontaneous effect Effects 0.000 description 4
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 3
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 description 3
- KDLHZDBZIXYQEI-UHFFFAOYSA-N Palladium Chemical compound [Pd] KDLHZDBZIXYQEI-UHFFFAOYSA-N 0.000 description 3
- WGLPBDUCMAPZCE-UHFFFAOYSA-N Trioxochromium Chemical compound O=[Cr](=O)=O WGLPBDUCMAPZCE-UHFFFAOYSA-N 0.000 description 3
- 229910000420 cerium oxide Inorganic materials 0.000 description 3
- 229910000423 chromium oxide Inorganic materials 0.000 description 3
- 238000002474 experimental method Methods 0.000 description 3
- 239000012528 membrane Substances 0.000 description 3
- 229910052751 metal Inorganic materials 0.000 description 3
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- 229910052757 nitrogen Inorganic materials 0.000 description 3
- 230000003647 oxidation Effects 0.000 description 3
- 238000007254 oxidation reaction Methods 0.000 description 3
- BMMGVYCKOGBVEV-UHFFFAOYSA-N oxo(oxoceriooxy)cerium Chemical compound [Ce]=O.O=[Ce]=O BMMGVYCKOGBVEV-UHFFFAOYSA-N 0.000 description 3
- 238000002161 passivation Methods 0.000 description 3
- 239000007858 starting material Substances 0.000 description 3
- NWUYHJFMYQTDRP-UHFFFAOYSA-N 1,2-bis(ethenyl)benzene;1-ethenyl-2-ethylbenzene;styrene Chemical compound C=CC1=CC=CC=C1.CCC1=CC=CC=C1C=C.C=CC1=CC=CC=C1C=C NWUYHJFMYQTDRP-UHFFFAOYSA-N 0.000 description 2
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 description 2
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 2
- UQSXHKLRYXJYBZ-UHFFFAOYSA-N Iron oxide Chemical compound [Fe]=O UQSXHKLRYXJYBZ-UHFFFAOYSA-N 0.000 description 2
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 description 2
- 150000001242 acetic acid derivatives Chemical class 0.000 description 2
- 230000004913 activation Effects 0.000 description 2
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 2
- 229910052788 barium Inorganic materials 0.000 description 2
- 238000001354 calcination Methods 0.000 description 2
- 229910052791 calcium Inorganic materials 0.000 description 2
- 150000004649 carbonic acid derivatives Chemical class 0.000 description 2
- 230000003197 catalytic effect Effects 0.000 description 2
- 150000001768 cations Chemical class 0.000 description 2
- 229910052804 chromium Inorganic materials 0.000 description 2
- PHFQLYPOURZARY-UHFFFAOYSA-N chromium trinitrate Chemical compound [Cr+3].[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O PHFQLYPOURZARY-UHFFFAOYSA-N 0.000 description 2
- 238000005868 electrolysis reaction Methods 0.000 description 2
- 229910002804 graphite Inorganic materials 0.000 description 2
- 239000010439 graphite Substances 0.000 description 2
- 238000010438 heat treatment Methods 0.000 description 2
- 238000005470 impregnation Methods 0.000 description 2
- 239000012535 impurity Substances 0.000 description 2
- 239000003456 ion exchange resin Substances 0.000 description 2
- 229920003303 ion-exchange polymer Polymers 0.000 description 2
- 229910052742 iron Inorganic materials 0.000 description 2
- 229910052747 lanthanoid Inorganic materials 0.000 description 2
- 150000002602 lanthanoids Chemical class 0.000 description 2
- 229910052746 lanthanum Inorganic materials 0.000 description 2
- 229910052749 magnesium Inorganic materials 0.000 description 2
- 229910021645 metal ion Inorganic materials 0.000 description 2
- 238000012544 monitoring process Methods 0.000 description 2
- 239000003345 natural gas Substances 0.000 description 2
- 230000001590 oxidative effect Effects 0.000 description 2
- 239000002245 particle Substances 0.000 description 2
- 229910052697 platinum Inorganic materials 0.000 description 2
- 239000010948 rhodium Substances 0.000 description 2
- 229910052706 scandium Inorganic materials 0.000 description 2
- 238000005245 sintering Methods 0.000 description 2
- 239000007787 solid Substances 0.000 description 2
- 239000000126 substance Substances 0.000 description 2
- 229910052717 sulfur Inorganic materials 0.000 description 2
- 239000011593 sulfur Substances 0.000 description 2
- 229910052727 yttrium Inorganic materials 0.000 description 2
- 239000004215 Carbon black (E152) Substances 0.000 description 1
- BVKZGUZCCUSVTD-UHFFFAOYSA-L Carbonate Chemical compound [O-]C([O-])=O BVKZGUZCCUSVTD-UHFFFAOYSA-L 0.000 description 1
- 229910052684 Cerium Inorganic materials 0.000 description 1
- VYZAMTAEIAYCRO-UHFFFAOYSA-N Chromium Chemical compound [Cr] VYZAMTAEIAYCRO-UHFFFAOYSA-N 0.000 description 1
- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 description 1
- 229910004298 SiO 2 Inorganic materials 0.000 description 1
- 229910010413 TiO 2 Inorganic materials 0.000 description 1
- GEIAQOFPUVMAGM-UHFFFAOYSA-N ZrO Inorganic materials [Zr]=O GEIAQOFPUVMAGM-UHFFFAOYSA-N 0.000 description 1
- PCBOWMZAEDDKNH-HOTGVXAUSA-N [4-(trifluoromethoxy)phenyl]methyl (3as,6as)-2-(3-fluoro-4-sulfamoylbenzoyl)-1,3,3a,4,6,6a-hexahydropyrrolo[3,4-c]pyrrole-5-carboxylate Chemical compound C1=C(F)C(S(=O)(=O)N)=CC=C1C(=O)N1C[C@H]2CN(C(=O)OCC=3C=CC(OC(F)(F)F)=CC=3)C[C@@H]2C1 PCBOWMZAEDDKNH-HOTGVXAUSA-N 0.000 description 1
- 239000004480 active ingredient Substances 0.000 description 1
- 229910000287 alkaline earth metal oxide Inorganic materials 0.000 description 1
- 229910021529 ammonia Inorganic materials 0.000 description 1
- 125000000129 anionic group Chemical group 0.000 description 1
- 239000012300 argon atmosphere Substances 0.000 description 1
- 239000002585 base Substances 0.000 description 1
- 239000003637 basic solution Substances 0.000 description 1
- 230000008901 benefit Effects 0.000 description 1
- 230000033228 biological regulation Effects 0.000 description 1
- 229910001593 boehmite Inorganic materials 0.000 description 1
- 230000000711 cancerogenic effect Effects 0.000 description 1
- 229910052799 carbon Inorganic materials 0.000 description 1
- 231100000315 carcinogenic Toxicity 0.000 description 1
- 238000006555 catalytic reaction Methods 0.000 description 1
- -1 cation nitrates Chemical class 0.000 description 1
- FFNYNHKYVBPMQP-UHFFFAOYSA-N cerium platinum Chemical compound [Ce].[Pt] FFNYNHKYVBPMQP-UHFFFAOYSA-N 0.000 description 1
- 238000001311 chemical methods and process Methods 0.000 description 1
- 239000007809 chemical reaction catalyst Substances 0.000 description 1
- 239000003638 chemical reducing agent Substances 0.000 description 1
- UPHIPHFJVNKLMR-UHFFFAOYSA-N chromium iron Chemical compound [Cr].[Fe] UPHIPHFJVNKLMR-UHFFFAOYSA-N 0.000 description 1
- 239000004927 clay Substances 0.000 description 1
- 239000011248 coating agent Substances 0.000 description 1
- 238000000576 coating method Methods 0.000 description 1
- 238000002485 combustion reaction Methods 0.000 description 1
- 238000007796 conventional method Methods 0.000 description 1
- TVZPLCNGKSPOJA-UHFFFAOYSA-N copper zinc Chemical compound [Cu].[Zn] TVZPLCNGKSPOJA-UHFFFAOYSA-N 0.000 description 1
- XTVVROIMIGLXTD-UHFFFAOYSA-N copper(II) nitrate Chemical compound [Cu+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O XTVVROIMIGLXTD-UHFFFAOYSA-N 0.000 description 1
- 230000006378 damage Effects 0.000 description 1
- 230000009849 deactivation Effects 0.000 description 1
- 230000003247 decreasing effect Effects 0.000 description 1
- 238000004455 differential thermal analysis Methods 0.000 description 1
- 238000001035 drying Methods 0.000 description 1
- 239000000428 dust Substances 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 239000003344 environmental pollutant Substances 0.000 description 1
- UQSQSQZYBQSBJZ-UHFFFAOYSA-N fluorosulfonic acid Chemical compound OS(F)(=O)=O UQSQSQZYBQSBJZ-UHFFFAOYSA-N 0.000 description 1
- 229910052733 gallium Inorganic materials 0.000 description 1
- 230000020169 heat generation Effects 0.000 description 1
- FAHBNUUHRFUEAI-UHFFFAOYSA-M hydroxidooxidoaluminium Chemical compound O[Al]=O FAHBNUUHRFUEAI-UHFFFAOYSA-M 0.000 description 1
- 229910052738 indium Inorganic materials 0.000 description 1
- 238000009776 industrial production Methods 0.000 description 1
- 239000007788 liquid Substances 0.000 description 1
- JCCNYMKQOSZNPW-UHFFFAOYSA-N loratadine Chemical compound C1CN(C(=O)OCC)CCC1=C1C2=NC=CC=C2CCC2=CC(Cl)=CC=C21 JCCNYMKQOSZNPW-UHFFFAOYSA-N 0.000 description 1
- 239000000314 lubricant Substances 0.000 description 1
- 229910052748 manganese Inorganic materials 0.000 description 1
- 238000010297 mechanical methods and process Methods 0.000 description 1
- 230000005226 mechanical processes and functions Effects 0.000 description 1
- 229910052759 nickel Inorganic materials 0.000 description 1
- 150000002823 nitrates Chemical class 0.000 description 1
- 229910017604 nitric acid Inorganic materials 0.000 description 1
- QJGQUHMNIGDVPM-UHFFFAOYSA-N nitrogen(.) Chemical compound [N] QJGQUHMNIGDVPM-UHFFFAOYSA-N 0.000 description 1
- 239000007800 oxidant agent Substances 0.000 description 1
- 229910052763 palladium Inorganic materials 0.000 description 1
- 239000008188 pellet Substances 0.000 description 1
- 231100000719 pollutant Toxicity 0.000 description 1
- 229920000642 polymer Polymers 0.000 description 1
- 239000005518 polymer electrolyte Substances 0.000 description 1
- 229910052573 porcelain Inorganic materials 0.000 description 1
- 239000000843 powder Substances 0.000 description 1
- 238000002360 preparation method Methods 0.000 description 1
- 230000003449 preventive effect Effects 0.000 description 1
- 238000012545 processing Methods 0.000 description 1
- 239000012495 reaction gas Substances 0.000 description 1
- 230000009467 reduction Effects 0.000 description 1
- 229910052703 rhodium Inorganic materials 0.000 description 1
- MHOVAHRLVXNVSD-UHFFFAOYSA-N rhodium atom Chemical compound [Rh] MHOVAHRLVXNVSD-UHFFFAOYSA-N 0.000 description 1
- 150000003839 salts Chemical class 0.000 description 1
- 230000000087 stabilizing effect Effects 0.000 description 1
- 238000010972 statistical evaluation Methods 0.000 description 1
- 238000000629 steam reforming Methods 0.000 description 1
- 238000003756 stirring Methods 0.000 description 1
- 239000004575 stone Substances 0.000 description 1
- 229910052712 strontium Inorganic materials 0.000 description 1
- 150000003467 sulfuric acid derivatives Chemical class 0.000 description 1
- 238000010998 test method Methods 0.000 description 1
- 230000009466 transformation Effects 0.000 description 1
- 238000000844 transformation Methods 0.000 description 1
- XJUNLJFOHNHSAR-UHFFFAOYSA-J zirconium(4+);dicarbonate Chemical compound [Zr+4].[O-]C([O-])=O.[O-]C([O-])=O XJUNLJFOHNHSAR-UHFFFAOYSA-J 0.000 description 1
Classifications
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M8/00—Fuel cells; Manufacture thereof
- H01M8/06—Combination of fuel cells with means for production of reactants or for treatment of residues
- H01M8/0662—Treatment of gaseous reactants or gaseous residues, e.g. cleaning
- H01M8/0668—Removal of carbon monoxide or carbon dioxide
-
- 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
- B01J23/76—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper combined with metals, oxides or hydroxides provided for in groups B01J23/02 - B01J23/36
- B01J23/80—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper combined with metals, oxides or hydroxides provided for in groups B01J23/02 - B01J23/36 with zinc, cadmium or mercury
-
- 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
- B01J37/00—Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
- B01J37/02—Impregnation, coating or precipitation
- B01J37/03—Precipitation; Co-precipitation
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- 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
- C01B3/06—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of inorganic compounds containing electro-positively bound hydrogen, e.g. water, acids, bases, ammonia, with inorganic reducing agents
- C01B3/12—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of inorganic compounds containing electro-positively bound hydrogen, e.g. water, acids, bases, ammonia, with inorganic reducing agents by reaction of water vapour with carbon monoxide
- C01B3/16—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of inorganic compounds containing electro-positively bound hydrogen, e.g. water, acids, bases, ammonia, with inorganic reducing agents by reaction of water vapour with carbon monoxide using catalysts
-
- 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
- B01J21/00—Catalysts comprising the elements, oxides, or hydroxides of magnesium, boron, aluminium, carbon, silicon, titanium, zirconium, or hafnium
- B01J21/06—Silicon, titanium, zirconium or hafnium; Oxides or hydroxides thereof
- B01J21/066—Zirconium or hafnium; Oxides or hydroxides thereof
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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
- B01J23/007—Mixed salts
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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
- B01J37/00—Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
- B01J37/0009—Use of binding agents; Moulding; Pressing; Powdering; Granulating; Addition of materials ameliorating the mechanical properties of the product catalyst
-
- 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
- C01B2203/10—Catalysts for performing the hydrogen forming reactions
- C01B2203/1041—Composition of the catalyst
- C01B2203/1076—Copper or zinc-based catalysts
-
- 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
- C01B2203/10—Catalysts for performing the hydrogen forming reactions
- C01B2203/1041—Composition of the catalyst
- C01B2203/1082—Composition of support materials
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M8/00—Fuel cells; Manufacture thereof
- H01M8/10—Fuel cells with solid electrolytes
- H01M2008/1095—Fuel cells with polymeric electrolytes
-
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Abstract
酸化銅、酸化亜鉛及び酸化アルミニウムを少なくとも含む混合酸化物を含み、その触媒前駆体が主としてハイドロタルサイトとして存在し、及び酸化銅含有量が20質量%以下であることを特徴とする触媒。
【選択図】なし
Description
MII 6MIII 2(OH)16CO3・4H2O
(但し、MIIが、少なくとも1種の二価の金属イオンであり、そして
MIIIが、少なくとも1種の三価の金属イオンである。)
のブルース石状の層を有している。
CuO:2〜20質量%、好ましくは4〜15質量%、特に好ましくは6〜12質量%;
ZnO:40〜80.5質量%、好ましくは50〜77質量%、特に好ましくは60〜75質量%;
Al2O3:17.5〜45質量%、好ましくは17.5〜35質量%、特に好ましくは17.5〜25質量%。
「雰囲気の変化」:運転(操作)温度で、運転ガス(CO、CO2、H2O、H2、N2)が遮断され、そして空気が触媒に通される。数分後、運転ガスが触媒に再び通される。
以下の組成:CuOが8質量%、ZnOが72質量%、Al2O3が17.5質量%、ZrO2が2.5質量%、を有する触媒の合成
1.031kgのCu硝酸塩溶液(19.4%濃度)、9.983kgのZn硝酸溶液(18.03%濃度)、及び5.388kgのAl硝酸塩溶液(8.12%濃度)を混合した(溶液1)。0.1462kgのZr炭酸塩を0.179kgのHNO3(69.3%濃度)に溶解した(溶液2)。溶液3を、2モルのNaOH及び0.3モルの炭酸ナトリウム溶液から作成した。溶液3を最初に挿入し、そして溶液1と溶液2を同時に挿入した。
以下の組成:CuOが8質量%、CeO2が15質量%、Cr2O3が2質量%、Al2O3が75質量%、を有する触媒の合成
WO02/26619A2、実施例2に記載したように、Al2O3球体DD−442を500℃に加熱した(表面積:230m2/g)。硝酸セリウム、硝酸クロム、及び硝酸銅を球体に連続的にスプレーし、そしてそれぞれの場合において、含浸の後、500℃でか焼した。
以下の組成:CuOが49質量%、ZnOが30質量%、Al2O3が18.5質量%、ZrO2が2.5質量%、を有する触媒の合成
Cu、Zn及びAlの硝酸塩溶液を、酸化物(質量%)の比が49:30:18.5で混合した。更に、炭酸ジルコニウムを、酸化物の比が2.5%で濃縮硝酸中に溶解した。水酸化ナトリウムと炭酸ナトリウムの混合溶液を作成した。溶液を組合せ、攪拌し、そして触媒前駆体を沈殿(析出)させた。次にサンプルを濾過、洗浄、乾燥し、550℃で4時間過熱し、そして実施例1.1に類似した方法で最終的にタブレット化した。
以下の組成:Al2O3上で、CuOが8質量%、CeO2が14質量%、を有する触媒の合成
SasolAl2O3球体を、磁製皿に置き、そして硝酸セリウムを滴下させて(攪拌させながら)加えた。含浸の後、球体を更に簡単に攪拌し、そして直ちに乾燥し、そしてか焼した。最初の工程と類似して、第2の工程では、球体をCu硝酸塩溶液で被覆した。各場合において、120℃で2時間、乾燥を行い、そしてマッフル炉中で、550℃でか焼を行った。
以下の組成:CuOが8%、ZnOが67%、Al2O3が17.5質量%、ZrO2が2.5質量%、Cr2O3が5質量%を有する触媒の合成
Cr硝酸塩溶液を(溶液1に)追加的に加え、そして実施例1.1の手順を行った。
以下の組成:CuOが8質量%、ZnOが89.5質量%、ZrO2が2.5質量%、を有する触媒の合成
もっぱらZn硝酸塩溶液から成る溶液1を使用し、実施例1.1の手順を行った。
最終組成:CuOが10質量%、ZnOが50質量%、Ce2O3が37.5質量%、ZrO2が2.5質量%
Al硝酸塩溶液の代わりにCe硝酸塩溶液を使用し、そして実施例1.1の手順を行った。
以下の組成:CuOが8%、ZnOが59.5%、Al2O3が30質量%(こものの13質%はVersalとして)、ZrO2が2.5質量%、を有する触媒の合成
Versalとして酸化アルミニウムの一部(13質量%)を加え、実施例1.1の手順を行った。
以下の組成:CuOが8質量%、ZnOが67質量%、Al2O3が17.5質量%、ZrO2が2.5質量%、Fe2O3が5質量%、を有する触媒の合成
(溶液1に)Fe硝酸塩溶液を加え、そして実施例1.1の手順を行った。
以下の組成:CuOが8質量%、ZnOが82質量%、Al2O3が7.5質量%、ZrO2が2.5質量%、を有する触媒の合成
実施例1.1に類似した方法を使用した。
以下の組成:CuOが8質量%、ZnOが74.5質量%、Al2O3が15質量%、ZrO2が2.5質量%、を有する触媒の合成
実施例1.1に類似した方法を使用した。
以下の組成:CuOが6質量%、ZnOが74質量%、Al2O3が17.5質量%、ZrO2が2.5質量%、を有する触媒の合成
実施例1.1に類似した方法を使用した。
以下の組成:CuOが10質量%、ZnOが70質量%、Al2O3が17.5質量%、ZrO2が2.5質量%、を有する触媒の合成
実施例1.1に類似した方法を使用した。
以下の組成:CuOが12質量%、ZnOが68質量%、Al2O3が17.5質量%、ZrO2が2.5質量%、を有する触媒の合成
実施例1.1に類似した方法を使用した。
加熱式反応器内に触媒を挿入した。反応器内に存在する活性銅の量が同一になるように体積を調節した。温度を上昇させ、水素の存在下に触媒を還元した。
実施例2.1で記載した装置内で、約200℃で、触媒における雰囲気の変更(切替)を(数回)行った。百分率は、オフガス(排ガス)中のCO濃度の変化を示す。従って、第1の触媒について、−20%は、雰囲気が変化した結果、雰囲気を変化させる前の値と比較して、CO濃度が20%低下したことを意味する。このことは、触媒が相当に活性化されていることを意味する。
実施例2.1に記載した装置内で、触媒上での水蒸気の凝縮を行った。次に触媒を(リフォーマット下に)130℃にし、そして実施例2.1に記載した温度勾配を施した。触媒が反応の平衡を達成する温度を測定した。
GHSVが5000h-1、及び以下のガス組成、COが8体積%、CO2が10体積%、H2が43体積%、H2Oが26体積%で、実施例2.1に類似した方法で、実験を行った。触媒は200℃で、熱力学的な平衡を達成した。
図2は、触媒1.1での代表的な測定曲線を示している。
図3は、触媒1.1での雰囲気の変化を示している。
実施例1.1に記載された方法で製造された、異なる組成を有するCu触媒の酸化で発生した熱の実験で、Cu含有量の関数としてプロットしている。
前駆体中のCuO含有量が12質量%未満の場合、触媒は自然発火しない範囲に存在する。
触媒1.1での代表的な測定曲線
触媒1.1での雰囲気の変化
三角形は、出口におけるCO濃度を示している(すう勢線を引いた)。
Claims (13)
- 一酸化炭素と水を水素と二酸化炭素に低温で変換するためのクロム非含有触媒であって、
酸化銅、酸化亜鉛及び酸化アルミニウムを少なくとも含む混合酸化物を含み、その触媒前駆体が、主としてハイドロタルサイトとして存在し、及び酸化銅含有量が20質量%以下であることを特徴とする触媒。 - 混合酸化物が、更に少なくとも1種の酸化ジルコニウムを含むことを特徴とする請求項1に記載の触媒。
- 貴金属を含まないことを特徴とする請求項1又は2の何れかに記載の触媒。
- 混合酸化物が、酸化銅を2〜20質量%、及び酸化亜鉛を40〜80.5質量%含むことを特徴とする請求項1〜3の何れか1項に記載の触媒。
- 混合酸化物が、酸化アルミニウムを45質量%以下で含むことを特徴とする請求項1〜4の何れか1項に記載の触媒。
- 混合酸化物が、酸化ジルコニウムを10質量%以下で含むことを特徴とする請求項1〜5の何れか1項に記載の触媒。
- 自然発火性でないことを特徴とする請求項1〜6の何れか1項に記載の触媒。
- 一酸化炭素と水とを水素と二酸化炭素に低温で変換するためのクロム非含有触媒を製造するための方法であって、
前記触媒は、少なくとも銅、亜鉛及びアルミニウムの化合物を含む前駆体物質から得られ、及び沈殿によって得られることを特徴とする方法。 - 前記沈殿は、塩基性媒体中で行われることを特徴とする請求項8に記載の方法。
- 炭酸ナトリウムと水酸化ナトリウムの混合物が使用されることを特徴とする請求項8又は9の何れかに記載の方法。
- 一酸化炭素と水とを二酸化炭素と水素に低温で変換する方法であって、
酸化銅、酸化亜鉛及び酸化アルミニウムを少なくとも含む混合酸化物を含み、酸化銅含有量が20質量%以下であり、及びその触媒前駆体が、主としてハイドロタルサイトとして存在するクロム非含有触媒が使用されることを特徴とする方法。 - 低温での変換が、150〜350℃の温度で行われることを特徴とする請求項11に記載の方法。
- 請求項11又は12に記載の方法によって製造された水素を燃料電池に使用する方法。
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JP2013529127A (ja) * | 2010-04-21 | 2013-07-18 | エスケー イノベーション カンパニー リミテッド | ナノメートルサイズの銅系触媒、その製造方法、及びそれを用いたカルボン酸の直接水素化によるアルコール製造方法 |
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JP5477561B2 (ja) * | 2009-09-09 | 2014-04-23 | 戸田工業株式会社 | 炭化水素を分解する多孔質触媒体及びその製造方法、炭化水素から水素を含む混合改質ガスを製造する方法、並びに燃料電池システム |
GB201015605D0 (en) | 2010-09-17 | 2010-10-27 | Magnesium Elektron Ltd | Inorganic oxides for co2 capture from exhaust systems |
CN103466546B (zh) * | 2013-09-06 | 2015-04-15 | 清华大学 | 一种将双功能吸附剂应用于吸附增强式水蒸气重整和水气变换反应的中温变压吸附方法 |
PL3368472T3 (pl) | 2015-10-29 | 2020-09-07 | Johnson Matthey Public Limited Company | Katalizator konwersji parowej tlenku węgla |
GB201519139D0 (en) | 2015-10-29 | 2015-12-16 | Johnson Matthey Plc | Process |
GB201519133D0 (en) | 2015-10-29 | 2015-12-16 | Johnson Matthey Plc | Process |
CN105833876B (zh) * | 2016-04-15 | 2019-03-26 | 西安向阳航天材料股份有限公司 | 一种高活性铜锌铝低温变换催化剂及其制备方法 |
EP3254760A1 (en) * | 2016-06-07 | 2017-12-13 | L'air Liquide, Societe Anonyme Pour L'etude Et L'exploitation Des Procedes Georges Claude | Process to synthesize a catalyst performing water-gas shift reaction at a high temperature |
CN109621967B (zh) * | 2018-12-26 | 2022-03-11 | 西安向阳航天材料股份有限公司 | 一种铜系低温变换催化剂的制备方法 |
CN114824320A (zh) * | 2022-03-07 | 2022-07-29 | 国网综合能源服务集团有限公司 | 一种具有铜包覆氧化锌界面的铜基催化剂的制备方法及其低温催化水煤气变换反应的应用 |
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