JP2012529135A - 電気化学用途の触媒 - Google Patents
電気化学用途の触媒 Download PDFInfo
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- JP2012529135A JP2012529135A JP2012513550A JP2012513550A JP2012529135A JP 2012529135 A JP2012529135 A JP 2012529135A JP 2012513550 A JP2012513550 A JP 2012513550A JP 2012513550 A JP2012513550 A JP 2012513550A JP 2012529135 A JP2012529135 A JP 2012529135A
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- catalyst
- transition metal
- platinum
- nickel
- alloy
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- 239000003054 catalyst Substances 0.000 title claims abstract description 169
- 229910052723 transition metal Inorganic materials 0.000 claims abstract description 47
- 238000001228 spectrum Methods 0.000 claims abstract description 44
- 150000003624 transition metals Chemical class 0.000 claims abstract description 42
- 238000010521 absorption reaction Methods 0.000 claims abstract description 20
- 238000000034 method Methods 0.000 claims abstract description 20
- 229910001260 Pt alloy Inorganic materials 0.000 claims abstract description 19
- 238000005259 measurement Methods 0.000 claims abstract description 18
- 239000003792 electrolyte Substances 0.000 claims abstract description 14
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims abstract description 13
- 239000001301 oxygen Substances 0.000 claims abstract description 13
- 229910052760 oxygen Inorganic materials 0.000 claims abstract description 13
- 238000006722 reduction reaction Methods 0.000 claims abstract description 12
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 claims description 128
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 claims description 74
- 229910052697 platinum Inorganic materials 0.000 claims description 52
- 239000000203 mixture Substances 0.000 claims description 30
- 229910045601 alloy Inorganic materials 0.000 claims description 29
- 239000000956 alloy Substances 0.000 claims description 29
- 239000000446 fuel Substances 0.000 claims description 22
- 229910052759 nickel Inorganic materials 0.000 claims description 22
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical group [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 19
- 229910052739 hydrogen Inorganic materials 0.000 claims description 19
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 claims description 17
- 229910052799 carbon Inorganic materials 0.000 claims description 17
- 239000001257 hydrogen Substances 0.000 claims description 17
- 239000013081 microcrystal Substances 0.000 claims description 6
- VYZAMTAEIAYCRO-UHFFFAOYSA-N Chromium Chemical compound [Cr] VYZAMTAEIAYCRO-UHFFFAOYSA-N 0.000 claims description 5
- 229910052804 chromium Inorganic materials 0.000 claims description 5
- 239000011651 chromium Substances 0.000 claims description 5
- 239000010941 cobalt Substances 0.000 claims description 5
- 229910017052 cobalt Inorganic materials 0.000 claims description 5
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 claims description 5
- 230000002441 reversible effect Effects 0.000 claims description 3
- 229910052720 vanadium Inorganic materials 0.000 claims description 3
- 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 2
- 238000000192 extended X-ray absorption fine structure spectroscopy Methods 0.000 claims 1
- LEONUFNNVUYDNQ-UHFFFAOYSA-N vanadium atom Chemical compound [V] LEONUFNNVUYDNQ-UHFFFAOYSA-N 0.000 claims 1
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 45
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- 239000002184 metal Substances 0.000 description 25
- 229910052757 nitrogen Inorganic materials 0.000 description 23
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- 239000008367 deionised water Substances 0.000 description 19
- 229910021641 deionized water Inorganic materials 0.000 description 19
- 239000007789 gas Substances 0.000 description 19
- 238000010438 heat treatment Methods 0.000 description 19
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 description 16
- NBIIXXVUZAFLBC-UHFFFAOYSA-N Phosphoric acid Chemical compound OP(O)(O)=O NBIIXXVUZAFLBC-UHFFFAOYSA-N 0.000 description 16
- QAOWNCQODCNURD-UHFFFAOYSA-N Sulfuric acid Chemical compound OS(O)(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-N 0.000 description 16
- 230000000694 effects Effects 0.000 description 13
- GNRSAWUEBMWBQH-UHFFFAOYSA-N oxonickel Chemical class [Ni]=O GNRSAWUEBMWBQH-UHFFFAOYSA-N 0.000 description 13
- 229910000480 nickel oxide Inorganic materials 0.000 description 12
- 239000000243 solution Substances 0.000 description 12
- 239000000463 material Substances 0.000 description 10
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 description 9
- 239000002253 acid Substances 0.000 description 9
- 229910000147 aluminium phosphate Inorganic materials 0.000 description 8
- 229910052786 argon Inorganic materials 0.000 description 8
- 239000010949 copper Substances 0.000 description 7
- 239000006185 dispersion Substances 0.000 description 7
- 239000012065 filter cake Substances 0.000 description 7
- 238000004519 manufacturing process Methods 0.000 description 7
- 239000002904 solvent Substances 0.000 description 7
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 6
- 150000001875 compounds Chemical class 0.000 description 6
- 238000009792 diffusion process Methods 0.000 description 6
- 238000001035 drying Methods 0.000 description 6
- 238000000921 elemental analysis Methods 0.000 description 6
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- QWPPOHNGKGFGJK-UHFFFAOYSA-N hypochlorous acid Chemical compound ClO QWPPOHNGKGFGJK-UHFFFAOYSA-N 0.000 description 6
- 239000012528 membrane Substances 0.000 description 6
- 238000002253 near-edge X-ray absorption fine structure spectrum Methods 0.000 description 6
- 239000002245 particle Substances 0.000 description 6
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- 239000002243 precursor Substances 0.000 description 6
- 239000002002 slurry Substances 0.000 description 6
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- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 5
- 238000006243 chemical reaction Methods 0.000 description 5
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- BFDHFSHZJLFAMC-UHFFFAOYSA-L nickel(ii) hydroxide Chemical compound [OH-].[OH-].[Ni+2] BFDHFSHZJLFAMC-UHFFFAOYSA-L 0.000 description 5
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- YRKCREAYFQTBPV-UHFFFAOYSA-N acetylacetone Chemical compound CC(=O)CC(C)=O YRKCREAYFQTBPV-UHFFFAOYSA-N 0.000 description 4
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- 230000008901 benefit Effects 0.000 description 4
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- 239000010411 electrocatalyst Substances 0.000 description 4
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- 230000008569 process Effects 0.000 description 4
- 229920006395 saturated elastomer Polymers 0.000 description 4
- 238000003756 stirring Methods 0.000 description 4
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 3
- RTZKZFJDLAIYFH-UHFFFAOYSA-N Diethyl ether Chemical compound CCOCC RTZKZFJDLAIYFH-UHFFFAOYSA-N 0.000 description 3
- WSFSSNUMVMOOMR-UHFFFAOYSA-N Formaldehyde Chemical compound O=C WSFSSNUMVMOOMR-UHFFFAOYSA-N 0.000 description 3
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 description 3
- 229910002837 PtCo Inorganic materials 0.000 description 3
- YXFVVABEGXRONW-UHFFFAOYSA-N Toluene Chemical compound CC1=CC=CC=C1 YXFVVABEGXRONW-UHFFFAOYSA-N 0.000 description 3
- 238000009835 boiling Methods 0.000 description 3
- 229910002091 carbon monoxide Inorganic materials 0.000 description 3
- 230000003197 catalytic effect Effects 0.000 description 3
- -1 chlorine ions Chemical class 0.000 description 3
- 230000000052 comparative effect Effects 0.000 description 3
- 150000002170 ethers Chemical class 0.000 description 3
- 238000009396 hybridization Methods 0.000 description 3
- 238000011065 in-situ storage Methods 0.000 description 3
- 239000011261 inert gas Substances 0.000 description 3
- 230000003993 interaction Effects 0.000 description 3
- VLKZOEOYAKHREP-UHFFFAOYSA-N n-Hexane Chemical compound CCCCCC VLKZOEOYAKHREP-UHFFFAOYSA-N 0.000 description 3
- BMGNSKKZFQMGDH-FDGPNNRMSA-L nickel(2+);(z)-4-oxopent-2-en-2-olate Chemical compound [Ni+2].C\C([O-])=C\C(C)=O.C\C([O-])=C\C(C)=O BMGNSKKZFQMGDH-FDGPNNRMSA-L 0.000 description 3
- 238000002161 passivation Methods 0.000 description 3
- 239000007787 solid Substances 0.000 description 3
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 2
- PWHULOQIROXLJO-UHFFFAOYSA-N Manganese Chemical compound [Mn] PWHULOQIROXLJO-UHFFFAOYSA-N 0.000 description 2
- JUJWROOIHBZHMG-UHFFFAOYSA-N Pyridine Chemical compound C1=CC=NC=C1 JUJWROOIHBZHMG-UHFFFAOYSA-N 0.000 description 2
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 2
- WYURNTSHIVDZCO-UHFFFAOYSA-N Tetrahydrofuran Chemical compound C1CCOC1 WYURNTSHIVDZCO-UHFFFAOYSA-N 0.000 description 2
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 description 2
- 238000002441 X-ray diffraction Methods 0.000 description 2
- 238000000862 absorption spectrum Methods 0.000 description 2
- 238000010306 acid treatment Methods 0.000 description 2
- 239000011149 active material Substances 0.000 description 2
- 125000004429 atom Chemical group 0.000 description 2
- 238000005229 chemical vapour deposition Methods 0.000 description 2
- FJDJVBXSSLDNJB-LNTINUHCSA-N cobalt;(z)-4-hydroxypent-3-en-2-one Chemical compound [Co].C\C(O)=C\C(C)=O.C\C(O)=C\C(C)=O.C\C(O)=C\C(C)=O FJDJVBXSSLDNJB-LNTINUHCSA-N 0.000 description 2
- 238000010924 continuous production Methods 0.000 description 2
- 238000005260 corrosion Methods 0.000 description 2
- 230000007797 corrosion Effects 0.000 description 2
- 230000005284 excitation Effects 0.000 description 2
- 239000011521 glass Substances 0.000 description 2
- 229910052500 inorganic mineral Inorganic materials 0.000 description 2
- 239000003446 ligand Substances 0.000 description 2
- 238000011068 loading method Methods 0.000 description 2
- 229910052748 manganese Inorganic materials 0.000 description 2
- 239000011572 manganese Substances 0.000 description 2
- 239000011707 mineral Substances 0.000 description 2
- VLTRZXGMWDSKGL-UHFFFAOYSA-N perchloric acid Chemical compound OCl(=O)(=O)=O VLTRZXGMWDSKGL-UHFFFAOYSA-N 0.000 description 2
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- 238000001556 precipitation Methods 0.000 description 2
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- 150000003839 salts Chemical class 0.000 description 2
- 239000002356 single layer Substances 0.000 description 2
- 239000000126 substance Substances 0.000 description 2
- GPPXJZIENCGNKB-UHFFFAOYSA-N vanadium Chemical compound [V]#[V] GPPXJZIENCGNKB-UHFFFAOYSA-N 0.000 description 2
- MFWFDRBPQDXFRC-LNTINUHCSA-N (z)-4-hydroxypent-3-en-2-one;vanadium Chemical compound [V].C\C(O)=C\C(C)=O.C\C(O)=C\C(C)=O.C\C(O)=C\C(C)=O MFWFDRBPQDXFRC-LNTINUHCSA-N 0.000 description 1
- POILWHVDKZOXJZ-ARJAWSKDSA-M (z)-4-oxopent-2-en-2-olate Chemical compound C\C([O-])=C\C(C)=O POILWHVDKZOXJZ-ARJAWSKDSA-M 0.000 description 1
- RYHBNJHYFVUHQT-UHFFFAOYSA-N 1,4-Dioxane Chemical compound C1COCCO1 RYHBNJHYFVUHQT-UHFFFAOYSA-N 0.000 description 1
- RMGHERXMTMUMMV-UHFFFAOYSA-N 2-methoxypropane Chemical compound COC(C)C RMGHERXMTMUMMV-UHFFFAOYSA-N 0.000 description 1
- DTIGTFJLLYWKTF-UHFFFAOYSA-N 2-methylnona-2,4-diene Chemical compound CCCCC=CC=C(C)C DTIGTFJLLYWKTF-UHFFFAOYSA-N 0.000 description 1
- BVKZGUZCCUSVTD-UHFFFAOYSA-M Bicarbonate Chemical compound OC([O-])=O BVKZGUZCCUSVTD-UHFFFAOYSA-M 0.000 description 1
- 229910000906 Bronze Inorganic materials 0.000 description 1
- VEXZGXHMUGYJMC-UHFFFAOYSA-M Chloride anion Chemical compound [Cl-] VEXZGXHMUGYJMC-UHFFFAOYSA-M 0.000 description 1
- XDTMQSROBMDMFD-UHFFFAOYSA-N Cyclohexane Chemical compound C1CCCCC1 XDTMQSROBMDMFD-UHFFFAOYSA-N 0.000 description 1
- ZOKXTWBITQBERF-UHFFFAOYSA-N Molybdenum Chemical compound [Mo] ZOKXTWBITQBERF-UHFFFAOYSA-N 0.000 description 1
- 229910003298 Ni-Ni Inorganic materials 0.000 description 1
- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 description 1
- 229910018553 Ni—O Inorganic materials 0.000 description 1
- 239000005922 Phosphane Substances 0.000 description 1
- XYFCBTPGUUZFHI-UHFFFAOYSA-N Phosphine Chemical compound P XYFCBTPGUUZFHI-UHFFFAOYSA-N 0.000 description 1
- KJTLSVCANCCWHF-UHFFFAOYSA-N Ruthenium Chemical compound [Ru] KJTLSVCANCCWHF-UHFFFAOYSA-N 0.000 description 1
- WGLPBDUCMAPZCE-UHFFFAOYSA-N Trioxochromium Chemical compound O=[Cr](=O)=O WGLPBDUCMAPZCE-UHFFFAOYSA-N 0.000 description 1
- 238000004998 X ray absorption near edge structure spectroscopy Methods 0.000 description 1
- 238000000833 X-ray absorption fine structure spectroscopy Methods 0.000 description 1
- MCMNRKCIXSYSNV-UHFFFAOYSA-N ZrO2 Inorganic materials O=[Zr]=O MCMNRKCIXSYSNV-UHFFFAOYSA-N 0.000 description 1
- YKIOKAURTKXMSB-UHFFFAOYSA-N adams's catalyst Chemical compound O=[Pt]=O YKIOKAURTKXMSB-UHFFFAOYSA-N 0.000 description 1
- 239000002156 adsorbate Substances 0.000 description 1
- 239000003513 alkali Substances 0.000 description 1
- 150000001336 alkenes Chemical class 0.000 description 1
- 239000008346 aqueous phase Substances 0.000 description 1
- 239000007864 aqueous solution Substances 0.000 description 1
- 239000012300 argon atmosphere Substances 0.000 description 1
- 150000001491 aromatic compounds Chemical class 0.000 description 1
- 239000002585 base Substances 0.000 description 1
- 238000010923 batch production Methods 0.000 description 1
- 239000010974 bronze Substances 0.000 description 1
- 239000002041 carbon nanotube Substances 0.000 description 1
- 229910021393 carbon nanotube Inorganic materials 0.000 description 1
- 125000002915 carbonyl group Chemical group [*:2]C([*:1])=O 0.000 description 1
- 239000000919 ceramic Substances 0.000 description 1
- 239000000460 chlorine Substances 0.000 description 1
- 229910052801 chlorine Inorganic materials 0.000 description 1
- 229910000423 chromium oxide Inorganic materials 0.000 description 1
- UFMZWBIQTDUYBN-UHFFFAOYSA-N cobalt dinitrate Chemical compound [Co+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O UFMZWBIQTDUYBN-UHFFFAOYSA-N 0.000 description 1
- 229910001981 cobalt nitrate Inorganic materials 0.000 description 1
- 150000004696 coordination complex Chemical class 0.000 description 1
- 229910000431 copper oxide Inorganic materials 0.000 description 1
- KUNSUQLRTQLHQQ-UHFFFAOYSA-N copper tin Chemical compound [Cu].[Sn] KUNSUQLRTQLHQQ-UHFFFAOYSA-N 0.000 description 1
- RKTYLMNFRDHKIL-UHFFFAOYSA-N copper;5,10,15,20-tetraphenylporphyrin-22,24-diide Chemical compound [Cu+2].C1=CC(C(=C2C=CC([N-]2)=C(C=2C=CC=CC=2)C=2C=CC(N=2)=C(C=2C=CC=CC=2)C2=CC=C3[N-]2)C=2C=CC=CC=2)=NC1=C3C1=CC=CC=C1 RKTYLMNFRDHKIL-UHFFFAOYSA-N 0.000 description 1
- 229960004643 cupric oxide Drugs 0.000 description 1
- 125000004093 cyano group Chemical group *C#N 0.000 description 1
- 150000004292 cyclic ethers Chemical class 0.000 description 1
- 238000000151 deposition Methods 0.000 description 1
- 230000008021 deposition Effects 0.000 description 1
- POLCUAVZOMRGSN-UHFFFAOYSA-N dipropyl ether Chemical compound CCCOCCC POLCUAVZOMRGSN-UHFFFAOYSA-N 0.000 description 1
- 238000009826 distribution Methods 0.000 description 1
- 238000004070 electrodeposition Methods 0.000 description 1
- 238000005868 electrolysis reaction Methods 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 239000008187 granular material Substances 0.000 description 1
- 239000010439 graphite Substances 0.000 description 1
- 229910002804 graphite Inorganic materials 0.000 description 1
- 150000002431 hydrogen Chemical class 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-M hydroxide Chemical compound [OH-] XLYOFNOQVPJJNP-UHFFFAOYSA-M 0.000 description 1
- 238000005470 impregnation Methods 0.000 description 1
- 230000010354 integration Effects 0.000 description 1
- 229910052742 iron Inorganic materials 0.000 description 1
- 125000002462 isocyano group Chemical group *[N+]#[C-] 0.000 description 1
- 239000003273 ketjen black Substances 0.000 description 1
- 239000010410 layer Substances 0.000 description 1
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- 150000001247 metal acetylides Chemical class 0.000 description 1
- 150000002736 metal compounds Chemical class 0.000 description 1
- 239000006082 mold release agent Substances 0.000 description 1
- 229910052750 molybdenum Inorganic materials 0.000 description 1
- 239000011733 molybdenum Substances 0.000 description 1
- 229910000476 molybdenum oxide Inorganic materials 0.000 description 1
- 229910017604 nitric acid Inorganic materials 0.000 description 1
- 150000004767 nitrides Chemical class 0.000 description 1
- 239000012299 nitrogen atmosphere Substances 0.000 description 1
- 229910000510 noble metal 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
- 238000010606 normalization Methods 0.000 description 1
- 150000002902 organometallic compounds Chemical class 0.000 description 1
- PQQKPALAQIIWST-UHFFFAOYSA-N oxomolybdenum Chemical compound [Mo]=O PQQKPALAQIIWST-UHFFFAOYSA-N 0.000 description 1
- RVTZCBVAJQQJTK-UHFFFAOYSA-N oxygen(2-);zirconium(4+) Chemical compound [O-2].[O-2].[Zr+4] RVTZCBVAJQQJTK-UHFFFAOYSA-N 0.000 description 1
- 230000037361 pathway Effects 0.000 description 1
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- 229910000064 phosphane Inorganic materials 0.000 description 1
- NBIIXXVUZAFLBC-UHFFFAOYSA-K phosphate Chemical compound [O-]P([O-])([O-])=O NBIIXXVUZAFLBC-UHFFFAOYSA-K 0.000 description 1
- 150000003057 platinum Chemical class 0.000 description 1
- NWAHZABTSDUXMJ-UHFFFAOYSA-N platinum(2+);dinitrate Chemical compound [Pt+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O NWAHZABTSDUXMJ-UHFFFAOYSA-N 0.000 description 1
- 239000002574 poison Substances 0.000 description 1
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- 239000005518 polymer electrolyte Substances 0.000 description 1
- 239000010970 precious metal Substances 0.000 description 1
- UMJSCPRVCHMLSP-UHFFFAOYSA-N pyridine Natural products COC1=CC=CN=C1 UMJSCPRVCHMLSP-UHFFFAOYSA-N 0.000 description 1
- 238000011002 quantification Methods 0.000 description 1
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- 229910052707 ruthenium Inorganic materials 0.000 description 1
- 238000000926 separation method Methods 0.000 description 1
- 239000000377 silicon dioxide Substances 0.000 description 1
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- 238000004611 spectroscopical analysis Methods 0.000 description 1
- YLQBMQCUIZJEEH-UHFFFAOYSA-N tetrahydrofuran Natural products C=1C=COC=1 YLQBMQCUIZJEEH-UHFFFAOYSA-N 0.000 description 1
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- WFKWXMTUELFFGS-UHFFFAOYSA-N tungsten Chemical compound [W] WFKWXMTUELFFGS-UHFFFAOYSA-N 0.000 description 1
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Images
Classifications
-
- 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
- B01J23/40—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals of the platinum group metals
- B01J23/42—Platinum
-
- 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
- B01J21/18—Carbon
-
- 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
- B01J23/89—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper combined with noble metals
-
- 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
- B01J23/89—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper combined with noble metals
- B01J23/8913—Cobalt and noble metals
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Abstract
Description
a)白金を含む触媒と遷移金属を含む熱分解性化合物とを混合して合金前駆体を得る工程、及び
b)該合金前駆体を還元性雰囲気下で加熱する工程
を含むプロセスによって製造することができる。
触媒の調製
技術(E−TEK)によるPtNi触媒
当該技術分野で公知のPtNi触媒は、例えば、WO−A−2006/056470号に記載されている。
本発明による合金触媒は好ましくは2段階の手順で製造される。最初に、担持されたPt触媒を製造する。次に、遷移金属成分をPt触媒で合金にする。
153.1gの炭素担体(Vulcan XC72、CABOT)を、Ultra−Turrax(登録商標)分散液装置(15分、8000rpm)によって5lの脱イオン水に分散させた。87.6gの硝酸白金(Heraeus、57.1質量%のPt)を1lの脱イオン水に溶解させ、追加の375mlの脱イオン水及び2125mlのエタノールをカーボン分散液に添加して、更に30分間撹拌した。反応混合物を次いで5時間加熱還流して室温まで冷却させる。得られた触媒分散液を濾過し、硝酸がなくなるまで(約30l)熱脱イオン水で洗浄する。濾過ケークを、残存水分量が35質量%になるまで空気中で乾燥させて、これを0.4mmの篩に通して粉砕する。
実施例1−PtNi(1)−(XANES、EXAFSのために使用される試料)
第1の工程で製造される38.5gの炭素担持白金触媒を、10.9gのニッケルアセチルアセトネートと混合し、これを連続運転可能な回転炉のリザーバーに導入する。回転炉を、リザーバーも含めて、アルゴンで1時間パージする(10l/時間)。
上で概説された方法に類似する手順で製造された63.4gの炭素担持白金触媒(乾燥量基準で30質量%のPt含有率、残留水分29質量%、即ち、「湿潤」触媒中21.3質量%のPt)を、23.0gのニッケルアセチルアセトネートと混合し、これを連続運転可能な回転炉のリザーバーに導入する。回転炉を、リザーバーも含めて、アルゴンで1時間パージする(10l/時間)。
第3の実施例では、非連続回転炉を使用する。
第1工程で製造される35.2gの炭素担持白金触媒を、11.1gのコバルトアセチルアセトネートと混合し、これを回転炉(HTM Reetz)に導入する。回転炉を窒素で1時間パージする(15l/時間)。
上で概説された方法と類似の手順で製造された18.0gの炭素担持白金触媒(23.2質量%Pt)を、8.9gのコバルトアセチルアセトネートと混合し、これを回転炉(HTM Reetz)に導入する。回転炉を窒素で1時間パージする(15l/時間)。
第1工程で製造される21.1gの炭素担持白金触媒を、10.5gのバナジウムアセチルアセトネートと混合し、これを回転炉(HTM Reetz)に導入する。回転炉を窒素で1時間パージする(15l/時間)。
Ni箔、NiO、及び水酸化ニッケルのXANESスペクトルを図1に示す。ニッケル箔(金属ニッケル)のスペクトルを実線1で示し、NiOのスペクトルを破線2で示し、水酸化ニッケルのスペクトルを白の三角形を有する破線3で示す。両方の酸化ニッケル化合物(酸化ニッケル及び水酸化ニッケル)が非常に類似したスペクトルを示すので、NiOのスペクトルのみが合金触媒を有する組成物のために使用されている。
触媒活性表面の測定のために、約15μg/cm2の触媒で被覆されているガラス炭素電極を、純粋な電解質(0.1MのHClO4)中で、0.05〜1.2Vの範囲で、10mV/sの走査速度で較正する。210μC/cm2の吸収された水素の単層に対する電荷量を考慮すると、白金表面は0.05〜0.4Vの間のピーク面積を積分することによって計算できる。その後、電極を、1mMのCuSO4を有する銅を含有する電解質(0.1MのHClO4)中で0.35Vで120秒間分極させる。最終的に、電極を10mV/sの走査速度で0.35V〜1.2Vの範囲で較正する。較正の間に銅を除去し、測定されている電流は、当初に吸収された銅の量に相当する。単層Cuの電荷密度(420μC/cm2)を考慮すると0.05〜0.4Vの間のピーク面積の積分は、触媒(白金及びニッケル)の全表面積の測定を可能にする。
触媒の触媒活性を酸素還元反応(ORR)に関して試験する。約15〜25μg/cm2の触媒で被覆されているガラス炭素電極を、HClO4(0.1又は1M)中で測定する。電極は1600rpmで回転している(回転ディスク電極、RDE)。アルゴン飽和電解質中で0〜0.95Vの間で測定した後、溶液を酸素で飽和し且つ0.05〜0.95Vの間で4つのシクロボルタモグラム(走査速度20mV/s)を記録する。活性度を0.9Vにて反応電流から測定し、これは0.9V(i0.9V)で測定された電流及び拡散限界電流(id)から計算されており、通常、以下の数式(質量比活性度):
Claims (12)
- 白金と遷移金属との合金を含む電気化学用途の触媒であって、前記遷移金属が、X線吸収端近傍スペクトル(XANES)によって測定された、酸化物状態の遷移金属の吸収端に類似する吸収端を有し、前記測定が濃H3PO4電解質中で行われる、前記触媒。
- 広域X線吸収微細構造(EXAFS)によって測定される遷移金属の結合距離が、酸化物状態の遷移金属の結合距離に相当する、請求項1に記載の触媒。
- 遷移金属がニッケル、クロム、バナジウム、コバルト、マンガン、及びそれらの混合物又は合金からなる群から選択される、請求項1に記載の触媒。
- 遷移金属に対する白金のモル比が1〜5の範囲である、請求項1に記載の触媒。
- 合金中の微結晶が5nm未満の平均サイズを有する、請求項1に記載の触媒。
- 触媒が更に担体を含む、請求項1に記載の触媒。
- 前記担体が炭素担体である、請求項6に記載の触媒。
- ニッケルの結合距離が1.5〜1.8Åの範囲である、請求項2に記載の触媒。
- 遷移金属がニッケルであり且つ測定が濃H3PO4電解質中で可逆水素電極に対して0.54Vで行われる、請求項1に記載の触媒。
- 請求項1に記載の触媒を電極触媒として使用する酸素還元反応の方法。
- 前記酸素還元反応を燃料電池中で行う、請求項10に記載の方法。
- 前記酸素還元反応を電解質としての濃H3PO4の存在下で行う、請求項10に記載の方法。
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WO2016063968A1 (ja) * | 2014-10-24 | 2016-04-28 | 株式会社キャタラー | 燃料電池用電極触媒及びその製造方法 |
JP2016209882A (ja) * | 2010-04-26 | 2016-12-15 | スリーエム イノベイティブ プロパティズ カンパニー | 白金ニッケル触媒合金 |
JPWO2017034029A1 (ja) * | 2015-08-27 | 2018-08-09 | 国立大学法人大阪大学 | 金属ナノ粒子製造方法、金属ナノ粒子担持担体製造方法、及び金属ナノ粒子担持担体 |
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CA2737629A1 (en) | 2008-09-18 | 2010-03-25 | Northeastern University | Platinum alloy electrocatalyst with enhanced resistance to anion poisoning for low and medium temperature fuel cells |
US9095845B2 (en) | 2010-10-21 | 2015-08-04 | Basf Se | Catalyst support material comprising polyazole salt, electrochemical catalyst, and the preparation of a gas diffusion electrode and a membrane-electrode assembly therefrom |
JP6008272B2 (ja) * | 2012-04-24 | 2016-10-19 | 国立大学法人名古屋大学 | 金属ナノクスラスター担持カーボン多孔体の製造方法 |
CN105655600A (zh) * | 2016-03-22 | 2016-06-08 | 陈波 | 一种Pt-Mn-石墨烯燃料电池催化剂的制备方法 |
KR20180013629A (ko) * | 2016-07-29 | 2018-02-07 | 에스케이하이닉스 주식회사 | 다층 자성 박막 스택 및 이를 포함하는 데이터 저장 장치 |
WO2019227340A1 (zh) * | 2018-05-30 | 2019-12-05 | 南方科技大学 | 金硫化镍核壳结构纳米电催化剂及其制备方法 |
KR102478160B1 (ko) * | 2019-10-30 | 2022-12-15 | 부산대학교 산학협력단 | 연료전지용 이종금속나노입자-탄소 혼성 촉매, 이의 제조방법 및 이를 포함하는 연료전지 |
CN112536042A (zh) * | 2020-11-19 | 2021-03-23 | 福州大学 | 一种甲醇催化氧化光电催化剂的制备方法 |
KR20220091754A (ko) * | 2020-12-24 | 2022-07-01 | 현대자동차주식회사 | 인터메탈릭 촉매 및 이의 제조 방법 |
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JPWO2017034029A1 (ja) * | 2015-08-27 | 2018-08-09 | 国立大学法人大阪大学 | 金属ナノ粒子製造方法、金属ナノ粒子担持担体製造方法、及び金属ナノ粒子担持担体 |
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WO2010139596A3 (en) | 2011-02-24 |
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EP2437883A2 (en) | 2012-04-11 |
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