JP5557831B2 - 燃料電池用触媒 - Google Patents
燃料電池用触媒 Download PDFInfo
- Publication number
- JP5557831B2 JP5557831B2 JP2011283458A JP2011283458A JP5557831B2 JP 5557831 B2 JP5557831 B2 JP 5557831B2 JP 2011283458 A JP2011283458 A JP 2011283458A JP 2011283458 A JP2011283458 A JP 2011283458A JP 5557831 B2 JP5557831 B2 JP 5557831B2
- Authority
- JP
- Japan
- Prior art keywords
- carbonitride
- laser
- fuel cell
- particles
- oxygen
- 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.)
- Expired - Fee Related
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- 239000000446 fuel Substances 0.000 title claims description 30
- 239000003054 catalyst Substances 0.000 title claims description 20
- 239000002245 particle Substances 0.000 claims description 124
- 239000000203 mixture Substances 0.000 claims description 106
- 239000012528 membrane Substances 0.000 claims description 10
- 239000011164 primary particle Substances 0.000 claims description 4
- 229910052723 transition metal Inorganic materials 0.000 claims description 4
- 150000003624 transition metals Chemical class 0.000 claims description 3
- 239000003792 electrolyte Substances 0.000 claims description 2
- 239000005518 polymer electrolyte Substances 0.000 claims description 2
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 75
- 229910052760 oxygen Inorganic materials 0.000 description 58
- 239000001301 oxygen Substances 0.000 description 58
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 57
- 238000006243 chemical reaction Methods 0.000 description 43
- 239000002994 raw material Substances 0.000 description 39
- 229910052757 nitrogen Inorganic materials 0.000 description 37
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 35
- 239000012159 carrier gas Substances 0.000 description 35
- 229910052799 carbon Inorganic materials 0.000 description 34
- 229910052751 metal Inorganic materials 0.000 description 32
- 239000002184 metal Substances 0.000 description 30
- 150000002736 metal compounds Chemical class 0.000 description 29
- 239000007789 gas Substances 0.000 description 25
- 238000004519 manufacturing process Methods 0.000 description 22
- 239000012495 reaction gas Substances 0.000 description 17
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 description 16
- 238000001725 laser pyrolysis Methods 0.000 description 16
- QCWXUUIWCKQGHC-UHFFFAOYSA-N Zirconium Chemical compound [Zr] QCWXUUIWCKQGHC-UHFFFAOYSA-N 0.000 description 14
- 229910052726 zirconium Inorganic materials 0.000 description 14
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 description 12
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 12
- 239000010936 titanium Substances 0.000 description 11
- 238000000034 method Methods 0.000 description 10
- WEVYAHXRMPXWCK-UHFFFAOYSA-N Acetonitrile Chemical compound CC#N WEVYAHXRMPXWCK-UHFFFAOYSA-N 0.000 description 9
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 description 9
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 description 9
- 229910052719 titanium Inorganic materials 0.000 description 9
- 229910021529 ammonia Inorganic materials 0.000 description 8
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 8
- 230000000052 comparative effect Effects 0.000 description 7
- 150000003839 salts Chemical class 0.000 description 7
- QTBSBXVTEAMEQO-UHFFFAOYSA-N Acetic acid Chemical compound CC(O)=O QTBSBXVTEAMEQO-UHFFFAOYSA-N 0.000 description 6
- CSCPPACGZOOCGX-UHFFFAOYSA-N Acetone Chemical compound CC(C)=O CSCPPACGZOOCGX-UHFFFAOYSA-N 0.000 description 6
- KFZMGEQAYNKOFK-UHFFFAOYSA-N Isopropanol Chemical compound CC(C)O KFZMGEQAYNKOFK-UHFFFAOYSA-N 0.000 description 6
- 229910052786 argon Inorganic materials 0.000 description 6
- 150000001875 compounds Chemical class 0.000 description 6
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 6
- 229910052758 niobium Inorganic materials 0.000 description 6
- 239000010955 niobium Substances 0.000 description 6
- GUCVJGMIXFAOAE-UHFFFAOYSA-N niobium atom Chemical compound [Nb] GUCVJGMIXFAOAE-UHFFFAOYSA-N 0.000 description 6
- -1 Carbon nitrides Chemical class 0.000 description 5
- 230000003197 catalytic effect Effects 0.000 description 5
- 238000009826 distribution Methods 0.000 description 5
- 150000002902 organometallic compounds Chemical class 0.000 description 5
- 239000000243 solution Substances 0.000 description 5
- 239000000126 substance Substances 0.000 description 5
- OHVLMTFVQDZYHP-UHFFFAOYSA-N 1-(2,4,6,7-tetrahydrotriazolo[4,5-c]pyridin-5-yl)-2-[4-[2-[[3-(trifluoromethoxy)phenyl]methylamino]pyrimidin-5-yl]piperazin-1-yl]ethanone Chemical compound N1N=NC=2CN(CCC=21)C(CN1CCN(CC1)C=1C=NC(=NC=1)NCC1=CC(=CC=C1)OC(F)(F)F)=O OHVLMTFVQDZYHP-UHFFFAOYSA-N 0.000 description 4
- LRHPLDYGYMQRHN-UHFFFAOYSA-N N-Butanol Chemical compound CCCCO LRHPLDYGYMQRHN-UHFFFAOYSA-N 0.000 description 4
- QAOWNCQODCNURD-UHFFFAOYSA-N Sulfuric acid Chemical compound OS(O)(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-N 0.000 description 4
- 239000012298 atmosphere Substances 0.000 description 4
- 239000006185 dispersion Substances 0.000 description 4
- BDAGIHXWWSANSR-UHFFFAOYSA-N methanoic acid Natural products OC=O BDAGIHXWWSANSR-UHFFFAOYSA-N 0.000 description 4
- 230000002194 synthesizing effect Effects 0.000 description 4
- VZSRBBMJRBPUNF-UHFFFAOYSA-N 2-(2,3-dihydro-1H-inden-2-ylamino)-N-[3-oxo-3-(2,4,6,7-tetrahydrotriazolo[4,5-c]pyridin-5-yl)propyl]pyrimidine-5-carboxamide Chemical compound C1C(CC2=CC=CC=C12)NC1=NC=C(C=N1)C(=O)NCCC(N1CC2=C(CC1)NN=N2)=O VZSRBBMJRBPUNF-UHFFFAOYSA-N 0.000 description 3
- WZFUQSJFWNHZHM-UHFFFAOYSA-N 2-[4-[2-(2,3-dihydro-1H-inden-2-ylamino)pyrimidin-5-yl]piperazin-1-yl]-1-(2,4,6,7-tetrahydrotriazolo[4,5-c]pyridin-5-yl)ethanone Chemical compound C1C(CC2=CC=CC=C12)NC1=NC=C(C=N1)N1CCN(CC1)CC(=O)N1CC2=C(CC1)NN=N2 WZFUQSJFWNHZHM-UHFFFAOYSA-N 0.000 description 3
- FIPWRIJSWJWJAI-UHFFFAOYSA-N Butyl carbitol 6-propylpiperonyl ether Chemical compound C1=C(CCC)C(COCCOCCOCCCC)=CC2=C1OCO2 FIPWRIJSWJWJAI-UHFFFAOYSA-N 0.000 description 3
- WSFSSNUMVMOOMR-UHFFFAOYSA-N Formaldehyde Chemical compound O=C WSFSSNUMVMOOMR-UHFFFAOYSA-N 0.000 description 3
- 238000002441 X-ray diffraction Methods 0.000 description 3
- 238000010521 absorption reaction Methods 0.000 description 3
- 238000010586 diagram Methods 0.000 description 3
- 238000010438 heat treatment Methods 0.000 description 3
- 239000001257 hydrogen Substances 0.000 description 3
- 229910052739 hydrogen Inorganic materials 0.000 description 3
- 239000000463 material Substances 0.000 description 3
- 229960005235 piperonyl butoxide Drugs 0.000 description 3
- IHCCLXNEEPMSIO-UHFFFAOYSA-N 2-[4-[2-(2,3-dihydro-1H-inden-2-ylamino)pyrimidin-5-yl]piperidin-1-yl]-1-(2,4,6,7-tetrahydrotriazolo[4,5-c]pyridin-5-yl)ethanone Chemical compound C1C(CC2=CC=CC=C12)NC1=NC=C(C=N1)C1CCN(CC1)CC(=O)N1CC2=C(CC1)NN=N2 IHCCLXNEEPMSIO-UHFFFAOYSA-N 0.000 description 2
- 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 2
- VGGSQFUCUMXWEO-UHFFFAOYSA-N Ethene Chemical compound C=C VGGSQFUCUMXWEO-UHFFFAOYSA-N 0.000 description 2
- 239000005977 Ethylene Substances 0.000 description 2
- AEMRFAOFKBGASW-UHFFFAOYSA-M Glycolate Chemical compound OCC([O-])=O AEMRFAOFKBGASW-UHFFFAOYSA-M 0.000 description 2
- OAKJQQAXSVQMHS-UHFFFAOYSA-N Hydrazine Chemical compound NN OAKJQQAXSVQMHS-UHFFFAOYSA-N 0.000 description 2
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 2
- AFCARXCZXQIEQB-UHFFFAOYSA-N N-[3-oxo-3-(2,4,6,7-tetrahydrotriazolo[4,5-c]pyridin-5-yl)propyl]-2-[[3-(trifluoromethoxy)phenyl]methylamino]pyrimidine-5-carboxamide Chemical compound O=C(CCNC(=O)C=1C=NC(=NC=1)NCC1=CC(=CC=C1)OC(F)(F)F)N1CC2=C(CC1)NN=N2 AFCARXCZXQIEQB-UHFFFAOYSA-N 0.000 description 2
- 229920000557 Nafion® Polymers 0.000 description 2
- GQPLMRYTRLFLPF-UHFFFAOYSA-N Nitrous Oxide Chemical compound [O-][N+]#N GQPLMRYTRLFLPF-UHFFFAOYSA-N 0.000 description 2
- ATUOYWHBWRKTHZ-UHFFFAOYSA-N Propane Chemical compound CCC ATUOYWHBWRKTHZ-UHFFFAOYSA-N 0.000 description 2
- MCMNRKCIXSYSNV-UHFFFAOYSA-N Zirconium dioxide Chemical compound O=[Zr]=O MCMNRKCIXSYSNV-UHFFFAOYSA-N 0.000 description 2
- IKHGUXGNUITLKF-XPULMUKRSA-N acetaldehyde Chemical compound [14CH]([14CH3])=O IKHGUXGNUITLKF-XPULMUKRSA-N 0.000 description 2
- 150000001298 alcohols Chemical class 0.000 description 2
- 150000001299 aldehydes Chemical class 0.000 description 2
- 150000004703 alkoxides Chemical class 0.000 description 2
- 238000009835 boiling Methods 0.000 description 2
- YHWCPXVTRSHPNY-UHFFFAOYSA-N butan-1-olate;titanium(4+) Chemical compound [Ti+4].CCCC[O-].CCCC[O-].CCCC[O-].CCCC[O-] YHWCPXVTRSHPNY-UHFFFAOYSA-N 0.000 description 2
- 239000006229 carbon black Substances 0.000 description 2
- 150000001735 carboxylic acids Chemical class 0.000 description 2
- 238000000576 coating method Methods 0.000 description 2
- 239000002131 composite material Substances 0.000 description 2
- 230000007423 decrease Effects 0.000 description 2
- 239000012776 electronic material Substances 0.000 description 2
- 238000000921 elemental analysis Methods 0.000 description 2
- UARGAUQGVANXCB-UHFFFAOYSA-N ethanol;zirconium Chemical compound [Zr].CCO.CCO.CCO.CCO UARGAUQGVANXCB-UHFFFAOYSA-N 0.000 description 2
- 235000019253 formic acid Nutrition 0.000 description 2
- 150000002576 ketones Chemical class 0.000 description 2
- 238000005259 measurement Methods 0.000 description 2
- ZTILUDNICMILKJ-UHFFFAOYSA-N niobium(v) ethoxide Chemical compound CCO[Nb](OCC)(OCC)(OCC)OCC ZTILUDNICMILKJ-UHFFFAOYSA-N 0.000 description 2
- 150000002825 nitriles Chemical class 0.000 description 2
- 239000012299 nitrogen atmosphere Substances 0.000 description 2
- MCCIMQKMMBVWHO-UHFFFAOYSA-N octadecanoic acid;titanium Chemical compound [Ti].CCCCCCCCCCCCCCCCCC(O)=O.CCCCCCCCCCCCCCCCCC(O)=O.CCCCCCCCCCCCCCCCCC(O)=O.CCCCCCCCCCCCCCCCCC(O)=O MCCIMQKMMBVWHO-UHFFFAOYSA-N 0.000 description 2
- JMANVNJQNLATNU-UHFFFAOYSA-N oxalonitrile Chemical compound N#CC#N JMANVNJQNLATNU-UHFFFAOYSA-N 0.000 description 2
- NFHFRUOZVGFOOS-UHFFFAOYSA-N palladium;triphenylphosphane Chemical compound [Pd].C1=CC=CC=C1P(C=1C=CC=CC=1)C1=CC=CC=C1.C1=CC=CC=C1P(C=1C=CC=CC=1)C1=CC=CC=C1.C1=CC=CC=C1P(C=1C=CC=CC=1)C1=CC=CC=C1.C1=CC=CC=C1P(C=1C=CC=CC=1)C1=CC=CC=C1 NFHFRUOZVGFOOS-UHFFFAOYSA-N 0.000 description 2
- BDERNNFJNOPAEC-UHFFFAOYSA-N propan-1-ol Chemical compound CCCO BDERNNFJNOPAEC-UHFFFAOYSA-N 0.000 description 2
- SBIBMFFZSBJNJF-UHFFFAOYSA-N selenium;zinc Chemical compound [Se]=[Zn] SBIBMFFZSBJNJF-UHFFFAOYSA-N 0.000 description 2
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N silicon dioxide Inorganic materials O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 2
- 239000006104 solid solution Substances 0.000 description 2
- 238000003786 synthesis reaction Methods 0.000 description 2
- JMXKSZRRTHPKDL-UHFFFAOYSA-N titanium ethoxide Chemical compound [Ti+4].CC[O-].CC[O-].CC[O-].CC[O-] JMXKSZRRTHPKDL-UHFFFAOYSA-N 0.000 description 2
- QDZRBIRIPNZRSG-UHFFFAOYSA-N titanium nitrate Chemical compound [O-][N+](=O)O[Ti](O[N+]([O-])=O)(O[N+]([O-])=O)O[N+]([O-])=O QDZRBIRIPNZRSG-UHFFFAOYSA-N 0.000 description 2
- XJDNKRIXUMDJCW-UHFFFAOYSA-J titanium tetrachloride Chemical compound Cl[Ti](Cl)(Cl)Cl XJDNKRIXUMDJCW-UHFFFAOYSA-J 0.000 description 2
- OERNJTNJEZOPIA-UHFFFAOYSA-N zirconium nitrate Chemical compound [Zr+4].[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O OERNJTNJEZOPIA-UHFFFAOYSA-N 0.000 description 2
- CGWDABYOHPEOAD-VIFPVBQESA-N (2r)-2-[(4-fluorophenoxy)methyl]oxirane Chemical compound C1=CC(F)=CC=C1OC[C@@H]1OC1 CGWDABYOHPEOAD-VIFPVBQESA-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
- CYWDDBNPXTUVNN-UHFFFAOYSA-I 2-ethylhexanoate;niobium(5+) Chemical compound [Nb+5].CCCCC(CC)C([O-])=O.CCCCC(CC)C([O-])=O.CCCCC(CC)C([O-])=O.CCCCC(CC)C([O-])=O.CCCCC(CC)C([O-])=O CYWDDBNPXTUVNN-UHFFFAOYSA-I 0.000 description 1
- AIFLGMNWQFPTAJ-UHFFFAOYSA-J 2-hydroxypropanoate;titanium(4+) Chemical compound [Ti+4].CC(O)C([O-])=O.CC(O)C([O-])=O.CC(O)C([O-])=O.CC(O)C([O-])=O AIFLGMNWQFPTAJ-UHFFFAOYSA-J 0.000 description 1
- SDTMFDGELKWGFT-UHFFFAOYSA-N 2-methylpropan-2-olate Chemical compound CC(C)(C)[O-] SDTMFDGELKWGFT-UHFFFAOYSA-N 0.000 description 1
- DUFCMRCMPHIFTR-UHFFFAOYSA-N 5-(dimethylsulfamoyl)-2-methylfuran-3-carboxylic acid Chemical compound CN(C)S(=O)(=O)C1=CC(C(O)=O)=C(C)O1 DUFCMRCMPHIFTR-UHFFFAOYSA-N 0.000 description 1
- HVGAPIUWXUVICC-UHFFFAOYSA-N 6-methylheptan-1-olate;titanium(4+) Chemical compound [Ti+4].CC(C)CCCCC[O-].CC(C)CCCCC[O-].CC(C)CCCCC[O-].CC(C)CCCCC[O-] HVGAPIUWXUVICC-UHFFFAOYSA-N 0.000 description 1
- 238000004438 BET method Methods 0.000 description 1
- 229910052582 BN Inorganic materials 0.000 description 1
- PZNSFCLAULLKQX-UHFFFAOYSA-N Boron nitride Chemical compound N#B PZNSFCLAULLKQX-UHFFFAOYSA-N 0.000 description 1
- BRHODLBZJKAKRN-UHFFFAOYSA-N C1=CC=CC1[Zr](C)(C)C1C=CC=C1 Chemical compound C1=CC=CC1[Zr](C)(C)C1C=CC=C1 BRHODLBZJKAKRN-UHFFFAOYSA-N 0.000 description 1
- KPWIZLJDXFLIAL-UHFFFAOYSA-L CC(C)O[Ti++]OC(C)C.CC(C)CCCCCCCCCCCCCCC([O-])=O.CC(C)CCCCCCCCCCCCCCC([O-])=O Chemical compound CC(C)O[Ti++]OC(C)C.CC(C)CCCCCCCCCCCCCCC([O-])=O.CC(C)CCCCCCCCCCCCCCC([O-])=O KPWIZLJDXFLIAL-UHFFFAOYSA-L 0.000 description 1
- DIICDKVONBLTBM-UHFFFAOYSA-L CC(C)O[Ti++]OC(C)C.CCCCCCCCCCCCCCCCCC([O-])=O.CCCCCCCCCCCCCCCCCC([O-])=O Chemical compound CC(C)O[Ti++]OC(C)C.CCCCCCCCCCCCCCCCCC([O-])=O.CCCCCCCCCCCCCCCCCC([O-])=O DIICDKVONBLTBM-UHFFFAOYSA-L 0.000 description 1
- KLQSRTKDOLFPQJ-UHFFFAOYSA-M CCCCO[Ti+](OCCCC)OCCCC.CCCCCCCCCCCCCCCCCC([O-])=O Chemical compound CCCCO[Ti+](OCCCC)OCCCC.CCCCCCCCCCCCCCCCCC([O-])=O KLQSRTKDOLFPQJ-UHFFFAOYSA-M 0.000 description 1
- GJEZUWLUOLSPJE-UHFFFAOYSA-N C[Ti](C)C Chemical compound C[Ti](C)C GJEZUWLUOLSPJE-UHFFFAOYSA-N 0.000 description 1
- FGPYCAFDFXYRLU-UHFFFAOYSA-N C[Zr](C1(C=CC=C1)C(C)(C)C)(C1(C=CC=C1)C(C)(C)C)C Chemical compound C[Zr](C1(C=CC=C1)C(C)(C)C)(C1(C=CC=C1)C(C)(C)C)C FGPYCAFDFXYRLU-UHFFFAOYSA-N 0.000 description 1
- JGPWYGYTHXNXRQ-UHFFFAOYSA-N Cl.Cl.Cl.C1C=CC=C1 Chemical compound Cl.Cl.Cl.C1C=CC=C1 JGPWYGYTHXNXRQ-UHFFFAOYSA-N 0.000 description 1
- OTMSDBZUPAUEDD-UHFFFAOYSA-N Ethane Chemical compound CC OTMSDBZUPAUEDD-UHFFFAOYSA-N 0.000 description 1
- NIPNSKYNPDTRPC-UHFFFAOYSA-N N-[2-oxo-2-(2,4,6,7-tetrahydrotriazolo[4,5-c]pyridin-5-yl)ethyl]-2-[[3-(trifluoromethoxy)phenyl]methylamino]pyrimidine-5-carboxamide Chemical compound O=C(CNC(=O)C=1C=NC(=NC=1)NCC1=CC(=CC=C1)OC(F)(F)F)N1CC2=C(CC1)NN=N2 NIPNSKYNPDTRPC-UHFFFAOYSA-N 0.000 description 1
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- CBENFWSGALASAD-UHFFFAOYSA-N Ozone Chemical compound [O-][O+]=O CBENFWSGALASAD-UHFFFAOYSA-N 0.000 description 1
- 229910018503 SF6 Inorganic materials 0.000 description 1
- BLRPTPMANUNPDV-UHFFFAOYSA-N Silane Chemical compound [SiH4] BLRPTPMANUNPDV-UHFFFAOYSA-N 0.000 description 1
- 235000010724 Wisteria floribunda Nutrition 0.000 description 1
- WYGQZDSIRBBVTA-UHFFFAOYSA-D [Nb+5].[Nb+5].[O-]C([O-])=O.[O-]C([O-])=O.[O-]C([O-])=O.[O-]C([O-])=O.[O-]C([O-])=O Chemical compound [Nb+5].[Nb+5].[O-]C([O-])=O.[O-]C([O-])=O.[O-]C([O-])=O.[O-]C([O-])=O.[O-]C([O-])=O WYGQZDSIRBBVTA-UHFFFAOYSA-D 0.000 description 1
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- BTVGHQASHWCGHI-UHFFFAOYSA-N acetic acid;butanoic acid Chemical compound CC(O)=O.CCCC(O)=O.CCCC(O)=O BTVGHQASHWCGHI-UHFFFAOYSA-N 0.000 description 1
- INNSZZHSFSFSGS-UHFFFAOYSA-N acetic acid;titanium Chemical compound [Ti].CC(O)=O.CC(O)=O.CC(O)=O.CC(O)=O INNSZZHSFSFSGS-UHFFFAOYSA-N 0.000 description 1
- 125000005595 acetylacetonate group Chemical group 0.000 description 1
- 125000000217 alkyl group Chemical group 0.000 description 1
- HSFWRNGVRCDJHI-UHFFFAOYSA-N alpha-acetylene Natural products C#C HSFWRNGVRCDJHI-UHFFFAOYSA-N 0.000 description 1
- 239000011324 bead Substances 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- METCOICSHWVCSX-UHFFFAOYSA-N bromo hypobromite niobium Chemical compound [Nb].BrOBr METCOICSHWVCSX-UHFFFAOYSA-N 0.000 description 1
- RQTQBQMVIJMUPB-UHFFFAOYSA-N butan-1-ol titanium Chemical compound [Ti].CCCCO.CCCCO.CCCCO RQTQBQMVIJMUPB-UHFFFAOYSA-N 0.000 description 1
- DINQVNXOZUORJS-UHFFFAOYSA-N butan-1-olate;niobium(5+) Chemical compound [Nb+5].CCCC[O-].CCCC[O-].CCCC[O-].CCCC[O-].CCCC[O-] DINQVNXOZUORJS-UHFFFAOYSA-N 0.000 description 1
- BSDOQSMQCZQLDV-UHFFFAOYSA-N butan-1-olate;zirconium(4+) Chemical compound [Zr+4].CCCC[O-].CCCC[O-].CCCC[O-].CCCC[O-] BSDOQSMQCZQLDV-UHFFFAOYSA-N 0.000 description 1
- RBSXMAJZDBCLHL-UHFFFAOYSA-L carbanide;dichloroniobium Chemical compound [CH3-].[CH3-].[CH3-].Cl[Nb]Cl RBSXMAJZDBCLHL-UHFFFAOYSA-L 0.000 description 1
- BVKZGUZCCUSVTD-UHFFFAOYSA-N carbonic acid Chemical compound OC(O)=O BVKZGUZCCUSVTD-UHFFFAOYSA-N 0.000 description 1
- 125000002915 carbonyl group Chemical group [*:2]C([*:1])=O 0.000 description 1
- XFVGXQSSXWIWIO-UHFFFAOYSA-N chloro hypochlorite;titanium Chemical compound [Ti].ClOCl XFVGXQSSXWIWIO-UHFFFAOYSA-N 0.000 description 1
- 239000011248 coating agent Substances 0.000 description 1
- 239000000470 constituent Substances 0.000 description 1
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- GKEMWFXJIFQMQF-UHFFFAOYSA-J cyclopentane;tetrachloroniobium Chemical compound [CH]1[CH][CH][CH][CH]1.Cl[Nb](Cl)(Cl)Cl GKEMWFXJIFQMQF-UHFFFAOYSA-J 0.000 description 1
- 238000000151 deposition Methods 0.000 description 1
- FNCWEPKWIKSHHW-UHFFFAOYSA-L dichloroniobium;methylcyclopentane Chemical compound Cl[Nb]Cl.C[C]1[CH][CH][CH][CH]1.C[C]1[CH][CH][CH][CH]1 FNCWEPKWIKSHHW-UHFFFAOYSA-L 0.000 description 1
- MIILMDFFARLWKZ-UHFFFAOYSA-L dichlorozirconium;1,2,3,4,5-pentamethylcyclopentane Chemical compound [Cl-].[Cl-].CC1=C(C)C(C)=C(C)C1(C)[Zr+2]C1(C)C(C)=C(C)C(C)=C1C MIILMDFFARLWKZ-UHFFFAOYSA-L 0.000 description 1
- LOKCKYUBKHNUCV-UHFFFAOYSA-L dichlorozirconium;methylcyclopentane Chemical compound Cl[Zr]Cl.C[C]1[CH][CH][CH][CH]1.C[C]1[CH][CH][CH][CH]1 LOKCKYUBKHNUCV-UHFFFAOYSA-L 0.000 description 1
- GOVWJRDDHRBJRW-UHFFFAOYSA-N diethylazanide;zirconium(4+) Chemical compound [Zr+4].CC[N-]CC.CC[N-]CC.CC[N-]CC.CC[N-]CC GOVWJRDDHRBJRW-UHFFFAOYSA-N 0.000 description 1
- 239000003085 diluting agent Substances 0.000 description 1
- 238000010790 dilution Methods 0.000 description 1
- 239000012895 dilution Substances 0.000 description 1
- 229910001873 dinitrogen Inorganic materials 0.000 description 1
- 238000010981 drying operation Methods 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- HHFAWKCIHAUFRX-UHFFFAOYSA-N ethoxide Chemical compound CC[O-] HHFAWKCIHAUFRX-UHFFFAOYSA-N 0.000 description 1
- SRLSISLWUNZOOB-UHFFFAOYSA-N ethyl(methyl)azanide;zirconium(4+) Chemical compound [Zr+4].CC[N-]C.CC[N-]C.CC[N-]C.CC[N-]C SRLSISLWUNZOOB-UHFFFAOYSA-N 0.000 description 1
- 125000002534 ethynyl group Chemical group [H]C#C* 0.000 description 1
- 238000011156 evaluation Methods 0.000 description 1
- 238000010304 firing Methods 0.000 description 1
- 239000012530 fluid Substances 0.000 description 1
- 238000010574 gas phase reaction Methods 0.000 description 1
- 239000011521 glass Substances 0.000 description 1
- 229910021397 glassy carbon Inorganic materials 0.000 description 1
- 229910002804 graphite Inorganic materials 0.000 description 1
- 239000010439 graphite Substances 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
- 150000002431 hydrogen Chemical class 0.000 description 1
- BBNMHKYUJLSCJS-UHFFFAOYSA-N iodo hypoiodite niobium Chemical compound [Nb].IOI BBNMHKYUJLSCJS-UHFFFAOYSA-N 0.000 description 1
- JMCVTQFKRIYPDK-UHFFFAOYSA-N iodo hypoiodite titanium Chemical compound O(I)I.[Ti] JMCVTQFKRIYPDK-UHFFFAOYSA-N 0.000 description 1
- VAPBTOIXFSABND-UHFFFAOYSA-N iodo hypoiodite zirconium Chemical compound [Zr].IOI VAPBTOIXFSABND-UHFFFAOYSA-N 0.000 description 1
- 239000003014 ion exchange membrane Substances 0.000 description 1
- 239000007788 liquid Substances 0.000 description 1
- 239000002923 metal particle Substances 0.000 description 1
- 150000002739 metals Chemical class 0.000 description 1
- QSLMQGXOMLSFAW-UHFFFAOYSA-N methanidylbenzene;zirconium(4+) Chemical compound [Zr+4].[CH2-]C1=CC=CC=C1.[CH2-]C1=CC=CC=C1.[CH2-]C1=CC=CC=C1.[CH2-]C1=CC=CC=C1 QSLMQGXOMLSFAW-UHFFFAOYSA-N 0.000 description 1
- IJCCNPITMWRYRC-UHFFFAOYSA-N methanolate;niobium(5+) Chemical compound [Nb+5].[O-]C.[O-]C.[O-]C.[O-]C.[O-]C IJCCNPITMWRYRC-UHFFFAOYSA-N 0.000 description 1
- WSFSSNUMVMOOMR-NJFSPNSNSA-N methanone Chemical compound O=[14CH2] WSFSSNUMVMOOMR-NJFSPNSNSA-N 0.000 description 1
- 238000002156 mixing Methods 0.000 description 1
- 239000002105 nanoparticle Substances 0.000 description 1
- LDPWMGUFXYRDRG-UHFFFAOYSA-I niobium(5+) pentaacetate Chemical compound [Nb+5].CC([O-])=O.CC([O-])=O.CC([O-])=O.CC([O-])=O.CC([O-])=O LDPWMGUFXYRDRG-UHFFFAOYSA-I 0.000 description 1
- KUJRRRAEVBRSIW-UHFFFAOYSA-N niobium(5+) pentanitrate Chemical compound [Nb+5].[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O KUJRRRAEVBRSIW-UHFFFAOYSA-N 0.000 description 1
- IIDYTZRUUWUVQF-UHFFFAOYSA-D niobium(5+) pentasulfate Chemical compound [Nb+5].[Nb+5].[O-]S([O-])(=O)=O.[O-]S([O-])(=O)=O.[O-]S([O-])(=O)=O.[O-]S([O-])(=O)=O.[O-]S([O-])(=O)=O IIDYTZRUUWUVQF-UHFFFAOYSA-D 0.000 description 1
- ZCNDFHXTXLMYDM-UHFFFAOYSA-I niobium(5+);pentaphenoxide Chemical compound [Nb+5].[O-]C1=CC=CC=C1.[O-]C1=CC=CC=C1.[O-]C1=CC=CC=C1.[O-]C1=CC=CC=C1.[O-]C1=CC=CC=C1 ZCNDFHXTXLMYDM-UHFFFAOYSA-I 0.000 description 1
- DSYRJFDOOSKABR-UHFFFAOYSA-I niobium(v) bromide Chemical compound [Br-].[Br-].[Br-].[Br-].[Br-].[Nb+5] DSYRJFDOOSKABR-UHFFFAOYSA-I 0.000 description 1
- 238000005121 nitriding Methods 0.000 description 1
- QJGQUHMNIGDVPM-UHFFFAOYSA-N nitrogen group Chemical group [N] QJGQUHMNIGDVPM-UHFFFAOYSA-N 0.000 description 1
- 239000001272 nitrous oxide Substances 0.000 description 1
- 150000002894 organic compounds Chemical class 0.000 description 1
- 230000001590 oxidative effect Effects 0.000 description 1
- TWNQGVIAIRXVLR-UHFFFAOYSA-N oxo(oxoalumanyloxy)alumane Chemical compound O=[Al]O[Al]=O TWNQGVIAIRXVLR-UHFFFAOYSA-N 0.000 description 1
- CMOAHYOGLLEOGO-UHFFFAOYSA-N oxozirconium;dihydrochloride Chemical compound Cl.Cl.[Zr]=O CMOAHYOGLLEOGO-UHFFFAOYSA-N 0.000 description 1
- 150000002926 oxygen Chemical class 0.000 description 1
- 125000004430 oxygen atom Chemical group O* 0.000 description 1
- DCKVFVYPWDKYDN-UHFFFAOYSA-L oxygen(2-);titanium(4+);sulfate Chemical compound [O-2].[Ti+4].[O-]S([O-])(=O)=O DCKVFVYPWDKYDN-UHFFFAOYSA-L 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
- YHBDIEWMOMLKOO-UHFFFAOYSA-I pentachloroniobium Chemical compound Cl[Nb](Cl)(Cl)(Cl)Cl YHBDIEWMOMLKOO-UHFFFAOYSA-I 0.000 description 1
- FWIYBTVHGYLSAZ-UHFFFAOYSA-I pentaiodoniobium Chemical compound I[Nb](I)(I)(I)I FWIYBTVHGYLSAZ-UHFFFAOYSA-I 0.000 description 1
- SGNLDVYVSFANHW-UHFFFAOYSA-N pentane-2,4-dione;zirconium Chemical compound [Zr].CC(=O)CC(C)=O SGNLDVYVSFANHW-UHFFFAOYSA-N 0.000 description 1
- 239000011941 photocatalyst Substances 0.000 description 1
- 238000006068 polycondensation reaction Methods 0.000 description 1
- 239000000843 powder Substances 0.000 description 1
- IKNCGYCHMGNBCP-UHFFFAOYSA-N propan-1-olate Chemical compound CCC[O-] IKNCGYCHMGNBCP-UHFFFAOYSA-N 0.000 description 1
- HKJYVRJHDIPMQB-UHFFFAOYSA-N propan-1-olate;titanium(4+) Chemical compound CCCO[Ti](OCCC)(OCCC)OCCC HKJYVRJHDIPMQB-UHFFFAOYSA-N 0.000 description 1
- XPGAWFIWCWKDDL-UHFFFAOYSA-N propan-1-olate;zirconium(4+) Chemical compound [Zr+4].CCC[O-].CCC[O-].CCC[O-].CCC[O-] XPGAWFIWCWKDDL-UHFFFAOYSA-N 0.000 description 1
- 239000001294 propane Substances 0.000 description 1
- 239000002096 quantum dot Substances 0.000 description 1
- 239000010453 quartz Substances 0.000 description 1
- 230000009257 reactivity Effects 0.000 description 1
- 230000002441 reversible effect Effects 0.000 description 1
- 229910000077 silane Inorganic materials 0.000 description 1
- 239000007787 solid Substances 0.000 description 1
- 239000002904 solvent Substances 0.000 description 1
- SFZCNBIFKDRMGX-UHFFFAOYSA-N sulfur hexafluoride Chemical compound FS(F)(F)(F)(F)F SFZCNBIFKDRMGX-UHFFFAOYSA-N 0.000 description 1
- 229960000909 sulfur hexafluoride Drugs 0.000 description 1
- 239000013076 target substance Substances 0.000 description 1
- 229910000349 titanium oxysulfate Inorganic materials 0.000 description 1
- 229910000348 titanium sulfate Inorganic materials 0.000 description 1
- UBZYKBZMAMTNKW-UHFFFAOYSA-J titanium tetrabromide Chemical compound Br[Ti](Br)(Br)Br UBZYKBZMAMTNKW-UHFFFAOYSA-J 0.000 description 1
- NLLZTRMHNHVXJJ-UHFFFAOYSA-J titanium tetraiodide Chemical compound I[Ti](I)(I)I NLLZTRMHNHVXJJ-UHFFFAOYSA-J 0.000 description 1
- FOZHTJJTSSSURD-UHFFFAOYSA-J titanium(4+);dicarbonate Chemical compound [Ti+4].[O-]C([O-])=O.[O-]C([O-])=O FOZHTJJTSSSURD-UHFFFAOYSA-J 0.000 description 1
- 238000002834 transmittance Methods 0.000 description 1
- 229910001928 zirconium oxide Inorganic materials 0.000 description 1
- DUNKXUFBGCUVQW-UHFFFAOYSA-J zirconium tetrachloride Chemical compound Cl[Zr](Cl)(Cl)Cl DUNKXUFBGCUVQW-UHFFFAOYSA-J 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
- ZXAUZSQITFJWPS-UHFFFAOYSA-J zirconium(4+);disulfate Chemical compound [Zr+4].[O-]S([O-])(=O)=O.[O-]S([O-])(=O)=O ZXAUZSQITFJWPS-UHFFFAOYSA-J 0.000 description 1
- LSWWNKUULMMMIL-UHFFFAOYSA-J zirconium(iv) bromide Chemical compound Br[Zr](Br)(Br)Br LSWWNKUULMMMIL-UHFFFAOYSA-J 0.000 description 1
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Description
炭窒化物の製造方法としては、一般的に特許文献1に示された方法のような金属表面に炭窒化物を直接析出させる手法が知られている。しかしこの方法では、炭窒化物自体を粉体として得ることは困難であり、後工程で別の形状に加工することが難しい。
本発明は、たとえば以下の(1)〜(7)に関する。
(1)
平均1次粒子径1〜100nmで合成された炭窒化物混合物粒子または炭窒酸化物混合物粒子を含むことを特徴とする燃料電池用触媒。
(2)
炭窒化物混合物粒子および炭窒酸化物混合物粒子は、粒度分布の偏差が3nm以下であることを特徴とする(1)に記載の燃料電池用触媒。
(3)
さらに電子伝導性粒子を含むことを特徴とする(1)または(2)に記載の燃料電池用触媒。
(4)
燃料電池用触媒層と多孔質支持層とを有する電極であって、前記燃料電池用触媒層が(1)〜(3)のいずれかに記載の燃料電池用触媒を含むことを特徴とする電極。
(5)
カソードとアノードと前記カソードおよび前記アノードの間に配置された電解質膜とを有する膜電極接合体であって、前記カソードおよび/または前記アノードが(4)に記載の電極であることを特徴とする膜電極接合体。
(6)
(5)に記載の膜電極接合体を備えることを特徴とする燃料電池。
(7)
(5)に記載の膜電極接合体を備えることを特徴とする固体高分子形燃料電池。
但し、本発明は以下の実施形態の各々に限定されるものではなく、例えば、これら実施形態の構成要素同士を適宜組み合わせても良い。
ここで、簡易のために、炭窒化物金属の真密度は、同金属の炭化物の真密度で代用し、炭窒酸化物金属の真密度は、同金属の酸化物の真密度で代用した。
本発明の金属の炭窒化物混合物粒子または炭窒酸化物混合物粒子の製造方法は、4族または5族の遷移金属の有機金属化合物、金属塩またはそれらの混合物と窒素源、必要に応じて炭素源及び酸素源とを希釈ガスとともに混合して得られた反応ガスを加熱して当該金属の炭窒化物混合物粒子または炭窒酸化物混合物粒子を得る製造方法において、加熱の熱源としてレーザ光を用いることを特徴とする。この製造方法は、たとえば以下のようなレーザ熱分解装置を用いて実施することができる。
図1は、本発明の製造方法で使用するレーザ熱分解装置の一具体例の構成を模式的に示した図である。図1において、符号101はレーザ、102は集光レンズ、103はチャンバー、104はキャリアーガスおよび酸素源導入口、105は金属化合物原料および炭素源導入口、106は窒素源導入口、107は反応ガス導入口、108は生成物搬出口、109は反応部である。
ニオブについては、ニオブメトキシド、ニオブブトキシド、ニオブエトキシド、ニオブフェノキシド、二塩化ビス(メチルシクロペンタジエニル)ニオブ、四塩化シクロペンタジエニルニオブ、2−エチルヘキサン酸ニオブ、テトラキス(2,2,6,6-テトラメチル−3,5−ヘプタンジオナト)ニオブ、ジクロロトリメチルニオブ等の物質を用いることができ、これらの中でも原料コストと、炭素−金属元素のバランスの面から、ニオブのエトキシド、ニオブのブトキシドを用いることが望ましい。
図2は本発明の製造方法で使用されるレーザ熱分解装置の他の構成を模式的に示した図である。この装置は、熱源として2つのレーザ光を用いた装置である。図2において、符号201は第一のレーザ、202は第一の集光レンズ、203は第二のレーザ、204は第二の集光レンズ、205はチャンバー、206は第一のキャリアーガス導入口、207は金属化合物原料導入口、208は炭素源導入口、209は窒素源導入口、210は反応ガス導入口、211は第二のキャリアーガス導入口、212は酸素源導入口、213は反応性ガス導入口、214は生成物搬出口、215は第一の反応部、216は第二の反応部である。
図2においては、反応部215および反応部216に照射されるレーザ光として別々のレーザから発生されたレーザ光を用いているが、1台のレーザから発生したレーザ光を分岐させ、2つのレーザ光として使用してもかまわない。この場合に、出力を別個に調整するために、分岐後にアッテネーターを設置することが好ましい。図3に1台のレーザら発生したレーザ光を分岐した場合の模式図を示す。
図1に示したレーザ熱分解装置を用いて、以下の条件で炭窒化物混合物粒子の製造を行った。チャンバー容積0.1立方メートルのチャンバー内にキャリアーガスとして200℃に予熱した窒素を20000sccm(sccm=standard cubic centimeter per minute)、炭素源として200℃に予熱したメタンを1000sccm、窒素源として200℃に予熱したアンモニアを5000sccm、金属化合物原料として200℃に予熱した四塩化チタンを毎分2g(10.5mmol)流した。このときのチャンバー圧力は200Torrであった。
得られたサンプルの組成比はTi1.0C0.15N0.35であった。
図2に示したレーザ熱分解装置を用いて、以下の条件で炭窒化物混合物粒子の製造を行った。反応部を2箇所有するチャンバー容積0.2立方メートルのチャンバー内にキャリアーガスとして200℃に予熱した窒素を30000sccm、窒素源として200℃に予熱したアンモニアを7000sccm、金属化合物原料として200℃に予熱したをチタニウムエトキシドを毎分4g(17.5mmol)流した。
さらに、第二の反応部にキャリアーガスとして200℃に予熱した窒素を10000sccm、酸素源として水を毎分1g流した。CO2レーザ1100Wの出力で発生させたレーザ光を、集光レンズを用いて第二の反応部へ集光させた。
第二の反応部で生じたチタンを含む炭窒酸化物混合物粒子は、ドライポンプがつながれた搬出口へと捕集された。その結果、平均粒径15nmの炭窒酸化物混合物粒子を作成することができた。このときの粒径分散はσ=2nmであった。
図2に示したレーザ熱分解装置を用いて、以下の条件で炭窒化物混合物粒子の製造を行った。反応部を2箇所有するチャンバー容積0.2立方メートルのチャンバー内にキャリアーガスとして200℃に予熱した窒素を30000sccm、窒素源として200℃に予熱したアンモニアを21000sccm、金属化合物原料として200℃に予熱したニオブエトキシドを毎分6g(18.9mmol)流した。CO2レーザ1200Wの出力で発生させたレーザ光を、集光レンズを用いて第一の反応部へ集光させた。
第二の反応部で生じたニオブを含む炭窒酸化物混合物粒子は、ドライポンプがつながれた搬出口へと捕集された。その結果、平均粒径20nmの炭窒酸化物混合物粒子を作成することができた。このときの粒径分散はσ=3nmであった。
図2に示したレーザ熱分解装置を用いて、以下の条件で炭窒化物混合物粒子の製造を行った。反応部を2箇所有するチャンバー容積0.2立方メートルのチャンバー内にキャリアーガスとして200℃に予熱したアルゴンを30000sccm、窒素源として200℃に予熱したアンモニアを21000sccm、金属化合物原料として200℃に予熱したジルコニウムターシャリーブトキシドを毎分7g(18.2mmol)流した。CO2レーザ1200Wの出力で発生させたレーザ光を、集光レンズを用いて第一の反応部へ集光させた。
第二の反応部で生じたジルコニウムを含む炭窒酸化物混合物粒子は、ドライポンプがつながれた搬出口へと捕集された。その結果、平均粒径30nmの炭窒酸化物混合物粒子を作成することができた。このときの粒径分散はσ=2nmであった。
(実施例4−1)で合成されたジルコニウムを含む炭窒酸化物混合物粒子0.095gとカーボン(キャボット社製 XC−72)0.005gを、イソプロピルアルコール:純水=1:1の重量比で混合した溶液10gに入れ、超音波を照射して撹拌、縣濁して混合した。この混合物20μlをグラッシーカーボン電極(東海カーボン社製、径:5.2mm)に塗布し、120℃で1時間乾燥し、この塗布、乾燥の操作を3回繰り返した。さらに、ナフィオン(デュポン社 5%ナフィオン溶液(DE521))を10倍に純水で希釈したもの10μlを塗布し、120℃で1時間乾燥し、燃料電池用電極を得た。
(実施例4−3)酸素還元能の評価
(実施例4−2)で作製された燃料電池用電極の触媒能(酸素還元能)を以下の方法で評価した。
すなわち、酸素還元開始電位が高いほど、また、酸素還元電流が大きいほど、燃料電池用電極の触媒能(酸素還元能)が高いことを示す。
実施例4で作製した燃料電池用電極は、酸素還元開始電位が0.81V(vs.NHE)であり、高い酸素還元能を有することがわかった。
酸化ジルコニウム(和光純薬製)1.2gとカーボンブラック(XC72、キャボット製)をよく混合し、窒化ホウ素坩堝に投入し、黒鉛炉(ハイマルチ5000、富士電波工業製)を用いて窒素気流中で2000℃で3時間加熱を行い1.1gのジルコニウムを含む炭窒化物混合物を得た。得られた炭窒化物混合物を坩堝に乗せたまま内径60mmのシリコニット炉に導入し、アルゴン中で1000℃まで昇温した。昇温後該アルゴン中に対して1体積%となるように酸素を導入し、1000℃を一時間保った後、酸素の供給を止め、アルゴン下で徐冷したところ、1.1gのジルコニウムを含む炭窒酸化物混合物が得られた。この炭窒酸化物混合物の粒子径は600nmであった。
(実施例4−1)で合成されたジルコニウムを含む炭窒酸化物混合物粒子に変えて、(比較例1−1)で合成されたジルコニウムを含む炭窒酸化物混合物を用いたほかは、(実施例4−2)と同様な手法で燃料電池用電極を得た。
(実施例4−2)で作成された電極に変えて、(比較例1−2)で作成した電極を用いた以外は(実施例4−3)と同様な手法で酸素還元触媒能を評価した。
Claims (6)
- 平均1次粒子径1〜100nmで合成された4族または5族の遷移金属の炭窒化物混合物粒子または炭窒酸化物混合物粒子を含むことを特徴とする燃料電池用触媒。
- さらに電子伝導性粒子を含むことを特徴とする請求項1に記載の燃料電池用触媒。
- 燃料電池用触媒層と多孔質支持層とを有する電極であって、前記燃料電池用触媒層が請求項1または2に記載の燃料電池用触媒を含むことを特徴とする電極。
- カソードとアノードと前記カソードおよび前記アノードの間に配置された電解質膜とを有する膜電極接合体であって、前記カソードおよび/または前記アノードが請求項3に記載の電極であることを特徴とする膜電極接合体。
- 請求項4に記載の膜電極接合体を備えることを特徴とする燃料電池。
- 請求項4に記載の膜電極接合体を備えることを特徴とする固体高分子形燃料電池。
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