JP6672272B2 - 触媒 - Google Patents
触媒 Download PDFInfo
- Publication number
- JP6672272B2 JP6672272B2 JP2017513063A JP2017513063A JP6672272B2 JP 6672272 B2 JP6672272 B2 JP 6672272B2 JP 2017513063 A JP2017513063 A JP 2017513063A JP 2017513063 A JP2017513063 A JP 2017513063A JP 6672272 B2 JP6672272 B2 JP 6672272B2
- Authority
- JP
- Japan
- Prior art keywords
- catalyst
- oxide
- metal oxide
- layer
- iridium
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
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- 239000003054 catalyst Substances 0.000 title claims description 149
- 239000012528 membrane Substances 0.000 claims description 45
- 229910044991 metal oxide Inorganic materials 0.000 claims description 42
- 150000004706 metal oxides Chemical class 0.000 claims description 42
- 239000010411 electrocatalyst Substances 0.000 claims description 35
- 239000007789 gas Substances 0.000 claims description 34
- 239000002245 particle Substances 0.000 claims description 32
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims description 31
- HTXDPTMKBJXEOW-UHFFFAOYSA-N dioxoiridium Chemical compound O=[Ir]=O HTXDPTMKBJXEOW-UHFFFAOYSA-N 0.000 claims description 31
- 229910000457 iridium oxide Inorganic materials 0.000 claims description 31
- 239000001301 oxygen Substances 0.000 claims description 31
- 229910052760 oxygen Inorganic materials 0.000 claims description 31
- 238000009792 diffusion process Methods 0.000 claims description 30
- 239000000446 fuel Substances 0.000 claims description 27
- 239000000758 substrate Substances 0.000 claims description 24
- 238000000034 method Methods 0.000 claims description 23
- 239000002243 precursor Substances 0.000 claims description 22
- 239000000203 mixture Substances 0.000 claims description 21
- 238000006243 chemical reaction Methods 0.000 claims description 19
- 229910052751 metal Inorganic materials 0.000 claims description 16
- 239000002184 metal Substances 0.000 claims description 16
- 238000012546 transfer Methods 0.000 claims description 14
- 239000002904 solvent Substances 0.000 claims description 13
- AMWRITDGCCNYAT-UHFFFAOYSA-L hydroxy(oxo)manganese;manganese Chemical compound [Mn].O[Mn]=O.O[Mn]=O AMWRITDGCCNYAT-UHFFFAOYSA-L 0.000 claims description 12
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 claims description 11
- 238000005118 spray pyrolysis Methods 0.000 claims description 9
- 229910052741 iridium Inorganic materials 0.000 claims description 8
- GKOZUEZYRPOHIO-UHFFFAOYSA-N iridium atom Chemical compound [Ir] GKOZUEZYRPOHIO-UHFFFAOYSA-N 0.000 claims description 7
- BPUBBGLMJRNUCC-UHFFFAOYSA-N oxygen(2-);tantalum(5+) Chemical compound [O-2].[O-2].[O-2].[O-2].[O-2].[Ta+5].[Ta+5] BPUBBGLMJRNUCC-UHFFFAOYSA-N 0.000 claims description 6
- 229910001936 tantalum oxide Inorganic materials 0.000 claims description 6
- 229910000410 antimony oxide Inorganic materials 0.000 claims description 5
- 229910000484 niobium oxide Inorganic materials 0.000 claims description 5
- URLJKFSTXLNXLG-UHFFFAOYSA-N niobium(5+);oxygen(2-) Chemical compound [O-2].[O-2].[O-2].[O-2].[O-2].[Nb+5].[Nb+5] URLJKFSTXLNXLG-UHFFFAOYSA-N 0.000 claims description 5
- VTRUBDSFZJNXHI-UHFFFAOYSA-N oxoantimony Chemical compound [Sb]=O VTRUBDSFZJNXHI-UHFFFAOYSA-N 0.000 claims description 5
- OGIDPMRJRNCKJF-UHFFFAOYSA-N titanium oxide Inorganic materials [Ti]=O OGIDPMRJRNCKJF-UHFFFAOYSA-N 0.000 claims description 5
- 238000000137 annealing Methods 0.000 claims description 2
- 230000001737 promoting effect Effects 0.000 claims 3
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 description 28
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 20
- 239000000976 ink Substances 0.000 description 18
- 229910052799 carbon Inorganic materials 0.000 description 17
- 150000002500 ions Chemical class 0.000 description 16
- 239000001257 hydrogen Substances 0.000 description 12
- 229910052739 hydrogen Inorganic materials 0.000 description 12
- 229910052697 platinum Inorganic materials 0.000 description 12
- 239000000463 material Substances 0.000 description 11
- -1 methanol or ethanol Chemical compound 0.000 description 10
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 9
- 229920001343 polytetrafluoroethylene Polymers 0.000 description 9
- 239000004810 polytetrafluoroethylene Substances 0.000 description 9
- 230000000052 comparative effect Effects 0.000 description 7
- 238000011068 loading method Methods 0.000 description 7
- 239000012702 metal oxide precursor Substances 0.000 description 7
- 238000007254 oxidation reaction Methods 0.000 description 7
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 7
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 6
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 6
- MHAJPDPJQMAIIY-UHFFFAOYSA-N Hydrogen peroxide Chemical compound OO MHAJPDPJQMAIIY-UHFFFAOYSA-N 0.000 description 6
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 description 6
- YXFVVABEGXRONW-UHFFFAOYSA-N Toluene Chemical compound CC1=CC=CC=C1 YXFVVABEGXRONW-UHFFFAOYSA-N 0.000 description 6
- 239000011248 coating agent Substances 0.000 description 6
- 238000000576 coating method Methods 0.000 description 6
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 6
- 229920000642 polymer Polymers 0.000 description 6
- 230000000694 effects Effects 0.000 description 5
- 238000006722 reduction reaction Methods 0.000 description 5
- 229920000049 Carbon (fiber) Polymers 0.000 description 4
- KDLHZDBZIXYQEI-UHFFFAOYSA-N Palladium Chemical compound [Pd] KDLHZDBZIXYQEI-UHFFFAOYSA-N 0.000 description 4
- 239000006229 carbon black Substances 0.000 description 4
- 239000004917 carbon fiber Substances 0.000 description 4
- 230000006378 damage Effects 0.000 description 4
- 238000000354 decomposition reaction Methods 0.000 description 4
- 238000009826 distribution Methods 0.000 description 4
- 238000005868 electrolysis reaction Methods 0.000 description 4
- 238000010438 heat treatment Methods 0.000 description 4
- 238000005259 measurement Methods 0.000 description 4
- 230000003647 oxidation Effects 0.000 description 4
- 239000000376 reactant Substances 0.000 description 4
- 230000006798 recombination Effects 0.000 description 4
- 238000005215 recombination Methods 0.000 description 4
- 230000002441 reversible effect Effects 0.000 description 4
- 238000004627 transmission electron microscopy Methods 0.000 description 4
- QTBSBXVTEAMEQO-UHFFFAOYSA-N Acetic acid Chemical compound CC(O)=O QTBSBXVTEAMEQO-UHFFFAOYSA-N 0.000 description 3
- WEVYAHXRMPXWCK-UHFFFAOYSA-N Acetonitrile Chemical compound CC#N WEVYAHXRMPXWCK-UHFFFAOYSA-N 0.000 description 3
- WVDDGKGOMKODPV-UHFFFAOYSA-N Benzyl alcohol Chemical compound OCC1=CC=CC=C1 WVDDGKGOMKODPV-UHFFFAOYSA-N 0.000 description 3
- KJTLSVCANCCWHF-UHFFFAOYSA-N Ruthenium Chemical compound [Ru] KJTLSVCANCCWHF-UHFFFAOYSA-N 0.000 description 3
- 229910000420 cerium oxide Inorganic materials 0.000 description 3
- 230000007797 corrosion Effects 0.000 description 3
- 238000005260 corrosion Methods 0.000 description 3
- 238000003487 electrochemical reaction Methods 0.000 description 3
- 239000003792 electrolyte Substances 0.000 description 3
- 238000006056 electrooxidation reaction Methods 0.000 description 3
- 239000004744 fabric Substances 0.000 description 3
- 150000002431 hydrogen Chemical class 0.000 description 3
- 230000002209 hydrophobic effect Effects 0.000 description 3
- 150000002739 metals Chemical class 0.000 description 3
- 239000002105 nanoparticle Substances 0.000 description 3
- 229910052757 nitrogen Inorganic materials 0.000 description 3
- 230000001590 oxidative effect Effects 0.000 description 3
- BMMGVYCKOGBVEV-UHFFFAOYSA-N oxo(oxoceriooxy)cerium Chemical compound [Ce]=O.O=[Ce]=O BMMGVYCKOGBVEV-UHFFFAOYSA-N 0.000 description 3
- 239000011148 porous material Substances 0.000 description 3
- 238000002360 preparation method Methods 0.000 description 3
- 229910052707 ruthenium Inorganic materials 0.000 description 3
- OBETXYAYXDNJHR-UHFFFAOYSA-N 2-Ethylhexanoic acid Chemical compound CCCCC(CC)C(O)=O OBETXYAYXDNJHR-UHFFFAOYSA-N 0.000 description 2
- 239000004812 Fluorinated ethylene propylene Substances 0.000 description 2
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 2
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 2
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 2
- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 description 2
- MCMNRKCIXSYSNV-UHFFFAOYSA-N Zirconium dioxide Chemical compound O=[Zr]=O MCMNRKCIXSYSNV-UHFFFAOYSA-N 0.000 description 2
- 238000005275 alloying Methods 0.000 description 2
- 238000004458 analytical method Methods 0.000 description 2
- 239000010953 base metal Substances 0.000 description 2
- 239000007809 chemical reaction catalyst Substances 0.000 description 2
- 238000002485 combustion reaction Methods 0.000 description 2
- 229920001940 conductive polymer Polymers 0.000 description 2
- 238000000151 deposition Methods 0.000 description 2
- 239000006185 dispersion Substances 0.000 description 2
- 238000005516 engineering process Methods 0.000 description 2
- SHZIWNPUGXLXDT-UHFFFAOYSA-N ethyl hexanoate Chemical compound CCCCCC(=O)OCC SHZIWNPUGXLXDT-UHFFFAOYSA-N 0.000 description 2
- 229920000840 ethylene tetrafluoroethylene copolymer Polymers 0.000 description 2
- PCHJSUWPFVWCPO-UHFFFAOYSA-N gold Chemical compound [Au] PCHJSUWPFVWCPO-UHFFFAOYSA-N 0.000 description 2
- 229910052737 gold Inorganic materials 0.000 description 2
- 239000010931 gold Substances 0.000 description 2
- 239000010439 graphite Substances 0.000 description 2
- 229910002804 graphite Inorganic materials 0.000 description 2
- 229910000449 hafnium oxide Inorganic materials 0.000 description 2
- WIHZLLGSGQNAGK-UHFFFAOYSA-N hafnium(4+);oxygen(2-) Chemical compound [O-2].[O-2].[Hf+4] WIHZLLGSGQNAGK-UHFFFAOYSA-N 0.000 description 2
- 238000005470 impregnation Methods 0.000 description 2
- 230000001976 improved effect Effects 0.000 description 2
- 229920000554 ionomer Polymers 0.000 description 2
- MRELNEQAGSRDBK-UHFFFAOYSA-N lanthanum(3+);oxygen(2-) Chemical compound [O-2].[O-2].[O-2].[La+3].[La+3] MRELNEQAGSRDBK-UHFFFAOYSA-N 0.000 description 2
- 238000004949 mass spectrometry Methods 0.000 description 2
- BDAGIHXWWSANSR-UHFFFAOYSA-N methanoic acid Natural products OC=O BDAGIHXWWSANSR-UHFFFAOYSA-N 0.000 description 2
- 239000002121 nanofiber Substances 0.000 description 2
- 229910052758 niobium Inorganic materials 0.000 description 2
- 239000010955 niobium Substances 0.000 description 2
- GUCVJGMIXFAOAE-UHFFFAOYSA-N niobium atom Chemical compound [Nb] GUCVJGMIXFAOAE-UHFFFAOYSA-N 0.000 description 2
- 229910052762 osmium Inorganic materials 0.000 description 2
- SYQBFIAQOQZEGI-UHFFFAOYSA-N osmium atom Chemical compound [Os] SYQBFIAQOQZEGI-UHFFFAOYSA-N 0.000 description 2
- 239000007800 oxidant agent Substances 0.000 description 2
- 229910052763 palladium Inorganic materials 0.000 description 2
- 229920009441 perflouroethylene propylene Polymers 0.000 description 2
- 230000008569 process Effects 0.000 description 2
- 229910052703 rhodium Inorganic materials 0.000 description 2
- 239000010948 rhodium Substances 0.000 description 2
- MHOVAHRLVXNVSD-UHFFFAOYSA-N rhodium atom Chemical compound [Rh] MHOVAHRLVXNVSD-UHFFFAOYSA-N 0.000 description 2
- 238000007650 screen-printing Methods 0.000 description 2
- 229910052709 silver Inorganic materials 0.000 description 2
- 239000004332 silver Substances 0.000 description 2
- 239000007921 spray Substances 0.000 description 2
- 239000000126 substance Substances 0.000 description 2
- 239000011135 tin Substances 0.000 description 2
- 229910052720 vanadium Inorganic materials 0.000 description 2
- FRWYFWZENXDZMU-UHFFFAOYSA-N 2-iodoquinoline Chemical compound C1=CC=CC2=NC(I)=CC=C21 FRWYFWZENXDZMU-UHFFFAOYSA-N 0.000 description 1
- OSWFIVFLDKOXQC-UHFFFAOYSA-N 4-(3-methoxyphenyl)aniline Chemical compound COC1=CC=CC(C=2C=CC(N)=CC=2)=C1 OSWFIVFLDKOXQC-UHFFFAOYSA-N 0.000 description 1
- QTBSBXVTEAMEQO-UHFFFAOYSA-M Acetate Chemical compound CC([O-])=O QTBSBXVTEAMEQO-UHFFFAOYSA-M 0.000 description 1
- 229920003934 Aciplex® Polymers 0.000 description 1
- 229920003937 Aquivion® Polymers 0.000 description 1
- 238000004438 BET method Methods 0.000 description 1
- 239000004215 Carbon black (E152) Substances 0.000 description 1
- VYZAMTAEIAYCRO-UHFFFAOYSA-N Chromium Chemical compound [Cr] VYZAMTAEIAYCRO-UHFFFAOYSA-N 0.000 description 1
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 1
- 229920003935 Flemion® Polymers 0.000 description 1
- 229920000557 Nafion® Polymers 0.000 description 1
- CTQNGGLPUBDAKN-UHFFFAOYSA-N O-Xylene Chemical compound CC1=CC=CC=C1C CTQNGGLPUBDAKN-UHFFFAOYSA-N 0.000 description 1
- 229920001774 Perfluoroether Polymers 0.000 description 1
- 239000004693 Polybenzimidazole Substances 0.000 description 1
- 229910001260 Pt alloy Inorganic materials 0.000 description 1
- ATJFFYVFTNAWJD-UHFFFAOYSA-N Tin Chemical compound [Sn] ATJFFYVFTNAWJD-UHFFFAOYSA-N 0.000 description 1
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 description 1
- 238000002441 X-ray diffraction Methods 0.000 description 1
- HCHKCACWOHOZIP-UHFFFAOYSA-N Zinc Chemical compound [Zn] HCHKCACWOHOZIP-UHFFFAOYSA-N 0.000 description 1
- XHCLAFWTIXFWPH-UHFFFAOYSA-N [O-2].[O-2].[O-2].[O-2].[O-2].[V+5].[V+5] Chemical compound [O-2].[O-2].[O-2].[O-2].[O-2].[V+5].[V+5] XHCLAFWTIXFWPH-UHFFFAOYSA-N 0.000 description 1
- 239000006230 acetylene black Substances 0.000 description 1
- 239000002253 acid Substances 0.000 description 1
- 239000000654 additive Substances 0.000 description 1
- 229910003481 amorphous carbon Inorganic materials 0.000 description 1
- 239000003125 aqueous solvent Substances 0.000 description 1
- 238000003556 assay Methods 0.000 description 1
- 238000000498 ball milling Methods 0.000 description 1
- 235000019445 benzyl alcohol Nutrition 0.000 description 1
- LTPBRCUWZOMYOC-UHFFFAOYSA-N beryllium oxide Inorganic materials O=[Be] LTPBRCUWZOMYOC-UHFFFAOYSA-N 0.000 description 1
- 239000011127 biaxially oriented polypropylene Substances 0.000 description 1
- 239000011230 binding agent Substances 0.000 description 1
- 230000005540 biological transmission Effects 0.000 description 1
- 229910000416 bismuth oxide Inorganic materials 0.000 description 1
- 238000004364 calculation method Methods 0.000 description 1
- 239000003575 carbonaceous material Substances 0.000 description 1
- 239000000969 carrier Substances 0.000 description 1
- 230000015556 catabolic process Effects 0.000 description 1
- CETPSERCERDGAM-UHFFFAOYSA-N ceric oxide Chemical compound O=[Ce]=O CETPSERCERDGAM-UHFFFAOYSA-N 0.000 description 1
- 229910000422 cerium(IV) oxide Inorganic materials 0.000 description 1
- 229910052804 chromium Inorganic materials 0.000 description 1
- 239000011651 chromium Substances 0.000 description 1
- 229910017052 cobalt Inorganic materials 0.000 description 1
- 239000010941 cobalt Substances 0.000 description 1
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 description 1
- 239000004020 conductor Substances 0.000 description 1
- 239000000356 contaminant Substances 0.000 description 1
- 229920001577 copolymer Polymers 0.000 description 1
- 229910052802 copper Inorganic materials 0.000 description 1
- 239000010949 copper Substances 0.000 description 1
- 238000006731 degradation reaction Methods 0.000 description 1
- 230000006866 deterioration Effects 0.000 description 1
- TYIXMATWDRGMPF-UHFFFAOYSA-N dibismuth;oxygen(2-) Chemical compound [O-2].[O-2].[O-2].[Bi+3].[Bi+3] TYIXMATWDRGMPF-UHFFFAOYSA-N 0.000 description 1
- 230000005611 electricity Effects 0.000 description 1
- QHSJIZLJUFMIFP-UHFFFAOYSA-N ethene;1,1,2,2-tetrafluoroethene Chemical group C=C.FC(F)=C(F)F QHSJIZLJUFMIFP-UHFFFAOYSA-N 0.000 description 1
- HQQADJVZYDDRJT-UHFFFAOYSA-N ethene;prop-1-ene Chemical group C=C.CC=C HQQADJVZYDDRJT-UHFFFAOYSA-N 0.000 description 1
- HHFAWKCIHAUFRX-UHFFFAOYSA-N ethoxide Chemical compound CC[O-] HHFAWKCIHAUFRX-UHFFFAOYSA-N 0.000 description 1
- 238000002474 experimental method Methods 0.000 description 1
- 238000001125 extrusion Methods 0.000 description 1
- 239000010419 fine particle Substances 0.000 description 1
- 125000001153 fluoro group Chemical group F* 0.000 description 1
- 229920002313 fluoropolymer Polymers 0.000 description 1
- 239000004811 fluoropolymer Substances 0.000 description 1
- UQSQSQZYBQSBJZ-UHFFFAOYSA-N fluorosulfonic acid Chemical compound OS(F)(=O)=O UQSQSQZYBQSBJZ-UHFFFAOYSA-N 0.000 description 1
- 235000019253 formic acid Nutrition 0.000 description 1
- 238000009472 formulation Methods 0.000 description 1
- 238000007755 gap coating Methods 0.000 description 1
- 238000007756 gravure coating Methods 0.000 description 1
- 150000004820 halides Chemical class 0.000 description 1
- 229930195733 hydrocarbon Natural products 0.000 description 1
- 150000002430 hydrocarbons Chemical class 0.000 description 1
- 238000010348 incorporation Methods 0.000 description 1
- 239000011261 inert gas Substances 0.000 description 1
- 230000000977 initiatory effect Effects 0.000 description 1
- 238000007641 inkjet printing Methods 0.000 description 1
- 229910003480 inorganic solid Inorganic materials 0.000 description 1
- HLYTZTFNIRBLNA-LNTINUHCSA-K iridium(3+);(z)-4-oxopent-2-en-2-olate Chemical compound [Ir+3].C\C([O-])=C\C(C)=O.C\C([O-])=C\C(C)=O.C\C([O-])=C\C(C)=O HLYTZTFNIRBLNA-LNTINUHCSA-K 0.000 description 1
- KZLHPYLCKHJIMM-UHFFFAOYSA-K iridium(3+);triacetate Chemical compound [Ir+3].CC([O-])=O.CC([O-])=O.CC([O-])=O KZLHPYLCKHJIMM-UHFFFAOYSA-K 0.000 description 1
- 229910052742 iron Inorganic materials 0.000 description 1
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- 230000007246 mechanism Effects 0.000 description 1
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- 150000001247 metal acetylides Chemical class 0.000 description 1
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- 230000000116 mitigating effect Effects 0.000 description 1
- 238000002156 mixing Methods 0.000 description 1
- 239000002071 nanotube Substances 0.000 description 1
- 229910052759 nickel Inorganic materials 0.000 description 1
- QGLKJKCYBOYXKC-UHFFFAOYSA-N nonaoxidotritungsten Chemical compound O=[W]1(=O)O[W](=O)(=O)O[W](=O)(=O)O1 QGLKJKCYBOYXKC-UHFFFAOYSA-N 0.000 description 1
- 239000003960 organic solvent Substances 0.000 description 1
- 150000002902 organometallic compounds Chemical class 0.000 description 1
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- 230000002572 peristaltic effect Effects 0.000 description 1
- WVDDGKGOMKODPV-ZQBYOMGUSA-N phenyl(114C)methanol Chemical compound O[14CH2]C1=CC=CC=C1 WVDDGKGOMKODPV-ZQBYOMGUSA-N 0.000 description 1
- 239000004033 plastic Substances 0.000 description 1
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- 230000004044 response Effects 0.000 description 1
- 239000000377 silicon dioxide Substances 0.000 description 1
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- 239000000725 suspension Substances 0.000 description 1
- 229910052715 tantalum Inorganic materials 0.000 description 1
- GUVRBAGPIYLISA-UHFFFAOYSA-N tantalum atom Chemical compound [Ta] GUVRBAGPIYLISA-UHFFFAOYSA-N 0.000 description 1
- 238000012360 testing method Methods 0.000 description 1
- BFKJFAAPBSQJPD-UHFFFAOYSA-N tetrafluoroethene Chemical group FC(F)=C(F)F BFKJFAAPBSQJPD-UHFFFAOYSA-N 0.000 description 1
- 229920001187 thermosetting polymer Polymers 0.000 description 1
- 229910052718 tin Inorganic materials 0.000 description 1
- 229910052719 titanium Inorganic materials 0.000 description 1
- 239000010936 titanium Substances 0.000 description 1
- 229910052723 transition metal Inorganic materials 0.000 description 1
- 150000003624 transition metals Chemical class 0.000 description 1
- UONOETXJSWQNOL-UHFFFAOYSA-N tungsten carbide Chemical compound [W+]#[C-] UONOETXJSWQNOL-UHFFFAOYSA-N 0.000 description 1
- 229910001930 tungsten oxide Inorganic materials 0.000 description 1
- LEONUFNNVUYDNQ-UHFFFAOYSA-N vanadium atom Chemical compound [V] LEONUFNNVUYDNQ-UHFFFAOYSA-N 0.000 description 1
- 229910001935 vanadium oxide Inorganic materials 0.000 description 1
- 238000007704 wet chemistry method Methods 0.000 description 1
- 239000008096 xylene Substances 0.000 description 1
- 229910052725 zinc Inorganic materials 0.000 description 1
- 239000011701 zinc Substances 0.000 description 1
Images
Classifications
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
- H01M4/90—Selection of catalytic material
- H01M4/9016—Oxides, hydroxides or oxygenated metallic salts
-
- 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
- B01J21/063—Titanium; Oxides or hydroxides thereof
-
- 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
- B01J23/38—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals
- B01J23/54—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals combined with metals, oxides or hydroxides provided for in groups B01J23/02 - B01J23/36
- B01J23/56—Platinum group metals
- B01J23/64—Platinum group metals with arsenic, antimony, bismuth, vanadium, niobium, tantalum, polonium, chromium, molybdenum, tungsten, manganese, technetium or rhenium
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Description
(i)電解触媒層はガス拡散層に塗布されて、ガス拡散電極を形成しうる。ガス拡散電極は、イオン伝導性膜の両側に配置され、一緒に積層化されて、5層のMEAを形成する。
(ii)電解触媒層は、イオン伝導性膜の両面に塗布され、触媒でコーティングされたイオン伝導性膜を生成しうる。その後、ガス拡散層は、触媒でコーティングされたイオン伝導性膜の両面に塗布される。
(iii)MEAは、一方の面が電解触媒層でコーティングされたイオン伝導性膜、電極触媒層に隣接するガス拡散層、及びイオン伝導性膜の他方の面上のガス拡散電極から形成することができる。
(i)セル反転:燃料電池は、時折、アノードへの燃料供給の一時的な減少によってしばしば引き起こされる電圧反転(セルが反対の極性に付勢される)を被る。これは、その後、カソードにおける酸素還元反応よりも高い電位で発生するアノードにおける炭素の電気的酸化といった、電流の生成を維持するために生じる一時的な望ましくない電気化学反応を引き起こす。このようなセル反転状況において(たとえ極めて短い期間であっても)、炭素の酸化によりアノード構造が不可逆的に損傷を受け、それにより電解触媒担体が失われる可能性がある。
(ii)スタートアップ/シャットダウン:燃料電池がしばらくの間アイドリングしている場合、空気に由来する酸素がカソード側から膜を通って拡散し、アノード側に依然として存在する任意の残留水素が移動する可能性が十分にある。セルが再起動され、水素がアノード内に再導入されるときに、空気がアノードから完全にパージされるまで、水素/空気の混合組成が、セルを通って移動するフロントとして、短時間の間アノードに存在する。入口側で水素に富み、出口側で空気に富んだフロントの存在は、カソード側で炭素の電気的酸化を高電位で生じさせ、アノードの出口側で酸化還元に対する逆反応が生じるように、燃料電池内に内部電気化学電池を設定することができる。このようなスタートアップ状態では、カソード構造は、炭素の酸化に起因して不可逆的に損傷を受ける場合があり、ひいてはカソード触媒層構造の永久劣化を生じうる。同様に損傷を与える電気化学電池は、シャットダウンにおいても設定されうる。このようなプロセスは、システム緩和戦略を採用することにより、例えばシャットダウンの間に窒素のような不活性ガスでアノードのガス空間をパージすることにより、制限することが可能であるが、MEAによる解決策によりこのようなシステム複雑化の必要性は緩和される。
H2O−>1/2O2+2H++2e−
本発明の実施例1から7は、実験室スケールの火炎噴霧熱分解法のセットアップを用いて調製された。酸化イリジウム及び金属酸化物の前駆体物質(下記表1に示す)を、生成物の組成に従って混合し、溶媒(トルエン)に溶解した。前駆体混合物中の全体の最終的金属濃度は、全体を通じて0.15mol/lに一定に保った。調製されたままの溶液は安定であり、表1に示す供給速度でぜん動ポンプにより火炎噴霧熱分解装置の火炎中へと送達された。火炎は、中央噴霧送達、予混合円形支持炎及び円形シートガス送達からなっている。酸素は、分散ガスとして使用され、表1に示す速度で送達された。メタン(1.5l/分)と酸素(3.2l/分)の混合物が、内部ノズルに供給され、予混合炎を形成した。すべてのガス流量は、較正済みマスフローコントローラーにより制御された。
IrO2/Ta2O5を、国際公開第2011/021034号に記載されるものと類似の方法を用いて調製した。
実施例1から7及び比較実施例1の各々の比表面積(BET)の測定値を決定した。結果を表2に示す。
実施例1の平均粒子サイズ及びd90を、分析を助けるGatanのDigital Micrograpソフトウェアを用いる透過電子顕微鏡法(TEM)を用いて測定した。図1は、実施例1の粒度分布分析を示している。実施例2から7の平均粒子サイズは、TEMから10nmを下回ることが分かった。
触媒層は、本発明の触媒(実施例1から7又は比較実施例1)を含むインクを、防水炭素繊維ガス拡散基材(ガス拡散層)上の疎水性マイクロポーラス層に刷毛塗りすることにより調製された。触媒インクは、EP0731520に記載される技術に従って作製された。触媒層における本発明の触媒のローディングを表3に示す。
Claims (15)
- 燃料電池における酸素発生反応を促進するための、 酸化イリジウム及び金属酸化物(M酸化物)の粒子を含む触媒であって、金属酸化物が、第4族金属酸化物、第5族金属酸化物、第7族金属酸化物及び酸化アンチモンからなる群より選択され、触媒の表面積が≧50m2/gであり、酸化イリジウム及び金属酸化物の粒子がd90≦15nmを有する、触媒。
- 金属酸化物が、酸化タンタル、酸化チタン、酸化アンチモン、酸化マンガン及び酸化ニオブからなる群より選択される、請求項1に記載の触媒。
- 金属酸化物における金属に対するイリジウムの原子比率が80:20から40:60である、請求項1又は2に記載の触媒。
- 燃料電池における酸素発生反応を促進するための触媒であって、触媒の表面積が≧50m2/gであり、酸化イリジウム及び金属酸化物の粒子がd90≦15nmを有することを特徴とする、酸化イリジウム及び金属酸化物の粒子を含む、触媒。
- 燃料電池における酸素発生反応を促進するための、酸化イリジウム及び金属酸化物の粒子を含む触媒を調製するための方法であって、金属酸化物が、第4族金属酸化物、第5族金属酸化物、第7族金属酸化物及び酸化アンチモンからなる群より選択され、前記方法が、前駆体混合物を火炎噴霧熱分解に供することを含み、前駆体混合物が、溶媒、酸化イリジウム前駆体及び金属酸化物前駆体を含み、触媒の表面積が≧50m2/gである、方法。
- アニーリング工程をさらに含む、請求項5に記載の方法。
- 請求項1から4のいずれか一項に記載の触媒及び電解触媒を含む触媒層。
- ガス拡散層及び請求項7に記載の触媒層を含むガス拡散電極。
- イオン伝導性膜及び請求項7に記載の触媒層を含む触媒化膜。
- キャリア/転写基材及び請求項7に記載の触媒層を含む触媒化キャリア/転写基材。
- 請求項1から4のいずれか一項に記載の触媒、又は請求項7に記載の触媒層、又は請求項8に記載のガス拡散電極、又は請求項9に記載の触媒化膜を含む膜電極アセンブリ。
- 請求項1から4のいずれか一項に記載の触媒、請求項7に記載の触媒層、請求項8に記載のガス拡散電極、請求項9に記載の触媒化膜、又は請求項11に記載の膜電極アセンブリを含む、電気化学デバイス。
- 酸素発生反応を触媒するための、請求項1から4のいずれか一項に記載の触媒の使用。
- 電気化学デバイスにおける、請求項1から4のいずれか一項に記載の触媒の使用。
- 電気化学デバイスが、高い電気化学電位に曝される電極を有する燃料電池である、請求項14に記載の使用。
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GBGB1415846.3A GB201415846D0 (en) | 2014-09-08 | 2014-09-08 | Catalyst |
GB1415846.3 | 2014-09-08 | ||
PCT/GB2015/052584 WO2016038349A1 (en) | 2014-09-08 | 2015-09-08 | Catalyst |
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JP2017533084A JP2017533084A (ja) | 2017-11-09 |
JP2017533084A5 JP2017533084A5 (ja) | 2018-09-27 |
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JP6288473B2 (ja) * | 2015-10-20 | 2018-03-07 | 三菱重工環境・化学エンジニアリング株式会社 | 水素発生装置 |
GB201621963D0 (en) | 2016-12-22 | 2017-02-08 | Johnson Matthey Plc | Catalyst-coated membrane having a laminate structure |
DE102018205571A1 (de) * | 2018-03-29 | 2019-10-02 | Siemens Aktiengesellschaft | Gasdiffusionselektrode, eine Elektrolyseanordnung sowie ein Verfahren zum Betreiben einer Elektrolyseanlage |
WO2019200115A1 (en) * | 2018-04-11 | 2019-10-17 | University Of Delaware | Electrochemical generation of carbon-containing products from carbon dioxide and carbon monoxide |
WO2019240200A1 (ja) * | 2018-06-12 | 2019-12-19 | 国立研究開発法人科学技術振興機構 | 触媒及びその使用方法 |
KR102180882B1 (ko) * | 2018-09-12 | 2020-11-20 | 주식회사 보야스에너지 | 초음파 분무 열분해법을 이용한 수전해 촉매 합성방법 |
DE102019133872A1 (de) * | 2018-12-19 | 2020-06-25 | Friedrich-Alexander-Universität Erlangen-Nürnberg | Brennstoffzelle oder Elektrolyseur |
JP7401115B2 (ja) * | 2019-02-28 | 2023-12-19 | 国立研究開発法人科学技術振興機構 | 電極触媒およびアミン化合物の製造方法 |
JP7188188B2 (ja) * | 2019-02-28 | 2022-12-13 | 株式会社豊田中央研究所 | 酸化反応用電極及びそれを用いた電気化学反応装置 |
EP3748039A1 (de) | 2019-06-07 | 2020-12-09 | Hahn-Schickard-Gesellschaft für angewandte Forschung e.V. | Elektrisch leitfähige nanofasern für eine polymermembran-basierte elektrolyse |
CN110433803A (zh) * | 2019-08-12 | 2019-11-12 | 华南理工大学 | 一种用于电解质膜电解水或水蒸气的负载型催化剂及其制备方法 |
CN111962131B (zh) * | 2020-07-14 | 2021-06-22 | 广东省科学院稀有金属研究所 | 一种析氧电极用复合氧化物催化涂层及其制备方法 |
DE102020126794A1 (de) | 2020-10-13 | 2022-04-14 | Greenerity Gmbh | Brennstoffzellen-Membranelektrodenanordnung und Brennstoffzelle |
DE102020126796A1 (de) * | 2020-10-13 | 2022-04-14 | Greenerity Gmbh | Sauerstoffevolutionskatalysator, Herstellung und Verwendung desselben, Membranelektrodenanordnung und Brennstoffzelle bzw. Elektrolysezelle |
GB202110475D0 (en) | 2021-07-21 | 2021-09-01 | Johnson Matthey Fuel Cells Ltd | Oxygen evolution reaction catalyst |
CN113881962A (zh) * | 2021-10-28 | 2022-01-04 | 西安泰金工业电化学技术有限公司 | 一种高导电性Ir-Ta-Mn复合氧化物涂层阳极的制备方法 |
US20230132969A1 (en) * | 2021-10-29 | 2023-05-04 | Robert Bosch Gmbh | Membrane electrode assembly catalyst material |
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