JP5813627B2 - 燃料電池 - Google Patents
燃料電池 Download PDFInfo
- Publication number
- JP5813627B2 JP5813627B2 JP2012508225A JP2012508225A JP5813627B2 JP 5813627 B2 JP5813627 B2 JP 5813627B2 JP 2012508225 A JP2012508225 A JP 2012508225A JP 2012508225 A JP2012508225 A JP 2012508225A JP 5813627 B2 JP5813627 B2 JP 5813627B2
- Authority
- JP
- Japan
- Prior art keywords
- catalyst
- side electrode
- cobalt
- fuel
- 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
Links
- 239000000446 fuel Substances 0.000 title claims description 105
- 239000003054 catalyst Substances 0.000 claims description 115
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims description 68
- 239000001301 oxygen Substances 0.000 claims description 68
- 229910052760 oxygen Inorganic materials 0.000 claims description 68
- 150000004032 porphyrins Chemical class 0.000 claims description 59
- 229910052723 transition metal Inorganic materials 0.000 claims description 48
- 229910017052 cobalt Inorganic materials 0.000 claims description 47
- 239000010941 cobalt Substances 0.000 claims description 47
- 150000003624 transition metals Chemical class 0.000 claims description 47
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 claims description 46
- 229910052799 carbon Inorganic materials 0.000 claims description 44
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 42
- 239000002131 composite material Substances 0.000 claims description 24
- 150000001875 compounds Chemical class 0.000 claims description 23
- 239000003792 electrolyte Substances 0.000 claims description 22
- 238000002156 mixing Methods 0.000 claims description 21
- 229920000128 polypyrrole Polymers 0.000 claims description 12
- 150000001450 anions Chemical class 0.000 claims description 4
- KAESVJOAVNADME-UHFFFAOYSA-N Pyrrole Chemical compound C=1C=CNC=1 KAESVJOAVNADME-UHFFFAOYSA-N 0.000 description 28
- 238000004519 manufacturing process Methods 0.000 description 28
- 239000000843 powder Substances 0.000 description 26
- 239000002904 solvent Substances 0.000 description 24
- 238000000034 method Methods 0.000 description 23
- 239000006185 dispersion Substances 0.000 description 22
- 238000012360 testing method Methods 0.000 description 22
- 239000002245 particle Substances 0.000 description 21
- WYURNTSHIVDZCO-UHFFFAOYSA-N Tetrahydrofuran Chemical compound C1CCOC1 WYURNTSHIVDZCO-UHFFFAOYSA-N 0.000 description 20
- -1 tetrahydrofuran Chemical compound 0.000 description 20
- 239000000243 solution Substances 0.000 description 19
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 18
- BDERNNFJNOPAEC-UHFFFAOYSA-N propan-1-ol Chemical compound CCCO BDERNNFJNOPAEC-UHFFFAOYSA-N 0.000 description 17
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 15
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 description 15
- 238000003756 stirring Methods 0.000 description 15
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 14
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 14
- 239000007788 liquid Substances 0.000 description 12
- 239000000203 mixture Substances 0.000 description 12
- KWYUFKZDYYNOTN-UHFFFAOYSA-M Potassium hydroxide Chemical compound [OH-].[K+] KWYUFKZDYYNOTN-UHFFFAOYSA-M 0.000 description 11
- 238000010438 heat treatment Methods 0.000 description 11
- 238000010248 power generation Methods 0.000 description 11
- KFZMGEQAYNKOFK-UHFFFAOYSA-N Isopropanol Chemical compound CC(C)O KFZMGEQAYNKOFK-UHFFFAOYSA-N 0.000 description 10
- 239000007864 aqueous solution Substances 0.000 description 10
- YLQBMQCUIZJEEH-UHFFFAOYSA-N tetrahydrofuran Natural products C=1C=COC=1 YLQBMQCUIZJEEH-UHFFFAOYSA-N 0.000 description 10
- QTBSBXVTEAMEQO-UHFFFAOYSA-N Acetic acid Chemical compound CC(O)=O QTBSBXVTEAMEQO-UHFFFAOYSA-N 0.000 description 9
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 description 9
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical group [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 description 9
- 238000006116 polymerization reaction Methods 0.000 description 9
- 238000006243 chemical reaction Methods 0.000 description 8
- 238000006722 reduction reaction Methods 0.000 description 8
- 230000000052 comparative effect Effects 0.000 description 7
- 239000001257 hydrogen Substances 0.000 description 7
- 229910052739 hydrogen Inorganic materials 0.000 description 7
- 239000012279 sodium borohydride Substances 0.000 description 7
- 229910000033 sodium borohydride Inorganic materials 0.000 description 7
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 description 6
- OAKJQQAXSVQMHS-UHFFFAOYSA-N Hydrazine Chemical compound NN OAKJQQAXSVQMHS-UHFFFAOYSA-N 0.000 description 6
- MHAJPDPJQMAIIY-UHFFFAOYSA-N Hydrogen peroxide Chemical compound OO MHAJPDPJQMAIIY-UHFFFAOYSA-N 0.000 description 6
- KDLHZDBZIXYQEI-UHFFFAOYSA-N Palladium Chemical compound [Pd] KDLHZDBZIXYQEI-UHFFFAOYSA-N 0.000 description 6
- 239000003957 anion exchange resin Substances 0.000 description 6
- 230000015572 biosynthetic process Effects 0.000 description 6
- 239000003638 chemical reducing agent Substances 0.000 description 6
- 238000001035 drying Methods 0.000 description 6
- 230000000694 effects Effects 0.000 description 6
- 229910052759 nickel Inorganic materials 0.000 description 6
- 230000001590 oxidative effect Effects 0.000 description 6
- ZMXDDKWLCZADIW-UHFFFAOYSA-N N,N-Dimethylformamide Chemical compound CN(C)C=O ZMXDDKWLCZADIW-UHFFFAOYSA-N 0.000 description 5
- 239000007789 gas Substances 0.000 description 5
- 150000002431 hydrogen Chemical class 0.000 description 5
- 239000011148 porous material Substances 0.000 description 5
- 239000007787 solid Substances 0.000 description 5
- IAZDPXIOMUYVGZ-UHFFFAOYSA-N Dimethylsulphoxide Chemical compound CS(C)=O IAZDPXIOMUYVGZ-UHFFFAOYSA-N 0.000 description 4
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical group [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 4
- MUBZPKHOEPUJKR-UHFFFAOYSA-N Oxalic acid Chemical compound OC(=O)C(O)=O MUBZPKHOEPUJKR-UHFFFAOYSA-N 0.000 description 4
- 150000001298 alcohols Chemical class 0.000 description 4
- 239000003011 anion exchange membrane Substances 0.000 description 4
- 239000010949 copper Substances 0.000 description 4
- 239000010931 gold Substances 0.000 description 4
- 239000011259 mixed solution Substances 0.000 description 4
- 230000000737 periodic effect Effects 0.000 description 4
- 239000010948 rhodium Substances 0.000 description 4
- 150000003839 salts Chemical class 0.000 description 4
- NWZSZGALRFJKBT-KNIFDHDWSA-N (2s)-2,6-diaminohexanoic acid;(2s)-2-hydroxybutanedioic acid Chemical compound OC(=O)[C@@H](O)CC(O)=O.NCCCC[C@H](N)C(O)=O NWZSZGALRFJKBT-KNIFDHDWSA-N 0.000 description 3
- PJOJZHHAECOAFH-UHFFFAOYSA-N 5,10,15,20-tetrakis(4-methoxyphenyl)-21,23-dihydroporphyrin Chemical compound COc1ccc(cc1)-c1c2ccc(n2)c(-c2ccc(OC)cc2)c2ccc([nH]2)c(-c2ccc(OC)cc2)c2ccc(n2)c(-c2ccc(OC)cc2)c2ccc1[nH]2 PJOJZHHAECOAFH-UHFFFAOYSA-N 0.000 description 3
- WEVYAHXRMPXWCK-UHFFFAOYSA-N Acetonitrile Chemical compound CC#N WEVYAHXRMPXWCK-UHFFFAOYSA-N 0.000 description 3
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 3
- UHOVQNZJYSORNB-UHFFFAOYSA-N Benzene Chemical compound C1=CC=CC=C1 UHOVQNZJYSORNB-UHFFFAOYSA-N 0.000 description 3
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 3
- JUJWROOIHBZHMG-UHFFFAOYSA-N Pyridine Chemical compound C1=CC=NC=C1 JUJWROOIHBZHMG-UHFFFAOYSA-N 0.000 description 3
- 230000010757 Reduction Activity Effects 0.000 description 3
- YXFVVABEGXRONW-UHFFFAOYSA-N Toluene Chemical compound CC1=CC=CC=C1 YXFVVABEGXRONW-UHFFFAOYSA-N 0.000 description 3
- ZMANZCXQSJIPKH-UHFFFAOYSA-N Triethylamine Chemical compound CCN(CC)CC ZMANZCXQSJIPKH-UHFFFAOYSA-N 0.000 description 3
- 239000003513 alkali Substances 0.000 description 3
- 229910021529 ammonia Inorganic materials 0.000 description 3
- 238000005349 anion exchange Methods 0.000 description 3
- 150000002170 ethers Chemical class 0.000 description 3
- IKDUDTNKRLTJSI-UHFFFAOYSA-N hydrazine monohydrate Substances O.NN IKDUDTNKRLTJSI-UHFFFAOYSA-N 0.000 description 3
- RAXXELZNTBOGNW-UHFFFAOYSA-N imidazole Natural products C1=CNC=N1 RAXXELZNTBOGNW-UHFFFAOYSA-N 0.000 description 3
- 239000000178 monomer Substances 0.000 description 3
- 239000012299 nitrogen atmosphere Substances 0.000 description 3
- 238000007254 oxidation reaction Methods 0.000 description 3
- 229920000642 polymer Polymers 0.000 description 3
- 239000005518 polymer electrolyte Substances 0.000 description 3
- 239000000377 silicon dioxide Substances 0.000 description 3
- 239000007921 spray Substances 0.000 description 3
- 239000000126 substance Substances 0.000 description 3
- ZNBNBTIDJSKEAM-UHFFFAOYSA-N 4-[7-hydroxy-2-[5-[5-[6-hydroxy-6-(hydroxymethyl)-3,5-dimethyloxan-2-yl]-3-methyloxolan-2-yl]-5-methyloxolan-2-yl]-2,8-dimethyl-1,10-dioxaspiro[4.5]decan-9-yl]-2-methyl-3-propanoyloxypentanoic acid Chemical compound C1C(O)C(C)C(C(C)C(OC(=O)CC)C(C)C(O)=O)OC11OC(C)(C2OC(C)(CC2)C2C(CC(O2)C2C(CC(C)C(O)(CO)O2)C)C)CC1 ZNBNBTIDJSKEAM-UHFFFAOYSA-N 0.000 description 2
- FUSNOPLQVRUIIM-UHFFFAOYSA-N 4-amino-2-(4,4-dimethyl-2-oxoimidazolidin-1-yl)-n-[3-(trifluoromethyl)phenyl]pyrimidine-5-carboxamide Chemical compound O=C1NC(C)(C)CN1C(N=C1N)=NC=C1C(=O)NC1=CC=CC(C(F)(F)F)=C1 FUSNOPLQVRUIIM-UHFFFAOYSA-N 0.000 description 2
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 description 2
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 2
- LYCAIKOWRPUZTN-UHFFFAOYSA-N Ethylene glycol Chemical compound OCCO LYCAIKOWRPUZTN-UHFFFAOYSA-N 0.000 description 2
- AVXURJPOCDRRFD-UHFFFAOYSA-N Hydroxylamine Chemical compound ON AVXURJPOCDRRFD-UHFFFAOYSA-N 0.000 description 2
- FXHOOIRPVKKKFG-UHFFFAOYSA-N N,N-Dimethylacetamide Chemical compound CN(C)C(C)=O FXHOOIRPVKKKFG-UHFFFAOYSA-N 0.000 description 2
- SECXISVLQFMRJM-UHFFFAOYSA-N N-Methylpyrrolidone Chemical compound CN1CCCC1=O SECXISVLQFMRJM-UHFFFAOYSA-N 0.000 description 2
- 229920000557 Nafion® Polymers 0.000 description 2
- NBIIXXVUZAFLBC-UHFFFAOYSA-N Phosphoric acid Chemical compound OP(O)(O)=O NBIIXXVUZAFLBC-UHFFFAOYSA-N 0.000 description 2
- NQRYJNQNLNOLGT-UHFFFAOYSA-N Piperidine Chemical compound C1CCNCC1 NQRYJNQNLNOLGT-UHFFFAOYSA-N 0.000 description 2
- ATUOYWHBWRKTHZ-UHFFFAOYSA-N Propane Chemical compound CCC ATUOYWHBWRKTHZ-UHFFFAOYSA-N 0.000 description 2
- KJTLSVCANCCWHF-UHFFFAOYSA-N Ruthenium Chemical compound [Ru] KJTLSVCANCCWHF-UHFFFAOYSA-N 0.000 description 2
- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 description 2
- 239000002253 acid Substances 0.000 description 2
- 150000004945 aromatic hydrocarbons Chemical class 0.000 description 2
- 150000001721 carbon Chemical class 0.000 description 2
- 230000003197 catalytic effect Effects 0.000 description 2
- 239000011651 chromium Substances 0.000 description 2
- 238000000576 coating method Methods 0.000 description 2
- UFMZWBIQTDUYBN-UHFFFAOYSA-N cobalt dinitrate Chemical compound [Co+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O UFMZWBIQTDUYBN-UHFFFAOYSA-N 0.000 description 2
- 238000004891 communication Methods 0.000 description 2
- 229910052802 copper Inorganic materials 0.000 description 2
- 230000007423 decrease Effects 0.000 description 2
- 238000010586 diagram Methods 0.000 description 2
- 229910021485 fumed silica Inorganic materials 0.000 description 2
- 229910021397 glassy carbon Inorganic materials 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
- 239000012493 hydrazine sulfate Substances 0.000 description 2
- 229910000377 hydrazine sulfate Inorganic materials 0.000 description 2
- 229910000378 hydroxylammonium sulfate Inorganic materials 0.000 description 2
- 229910052741 iridium Inorganic materials 0.000 description 2
- GKOZUEZYRPOHIO-UHFFFAOYSA-N iridium atom Chemical compound [Ir] GKOZUEZYRPOHIO-UHFFFAOYSA-N 0.000 description 2
- 239000011572 manganese Substances 0.000 description 2
- 238000005259 measurement Methods 0.000 description 2
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 2
- 239000011812 mixed powder Substances 0.000 description 2
- 239000010955 niobium Substances 0.000 description 2
- 229910052757 nitrogen Inorganic materials 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
- 230000003647 oxidation Effects 0.000 description 2
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- 229910052703 rhodium Inorganic materials 0.000 description 2
- MHOVAHRLVXNVSD-UHFFFAOYSA-N rhodium atom Chemical compound [Rh] MHOVAHRLVXNVSD-UHFFFAOYSA-N 0.000 description 2
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- 239000010936 titanium Substances 0.000 description 2
- 238000011144 upstream manufacturing Methods 0.000 description 2
- DIIIISSCIXVANO-UHFFFAOYSA-N 1,2-Dimethylhydrazine Chemical compound CNNC DIIIISSCIXVANO-UHFFFAOYSA-N 0.000 description 1
- 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 1
- JIHQDMXYYFUGFV-UHFFFAOYSA-N 1,3,5-triazine Chemical compound C1=NC=NC=N1 JIHQDMXYYFUGFV-UHFFFAOYSA-N 0.000 description 1
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- 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 1
- DFGKGUXTPFWHIX-UHFFFAOYSA-N 6-[2-[4-[2-(2,3-dihydro-1H-inden-2-ylamino)pyrimidin-5-yl]piperazin-1-yl]acetyl]-3H-1,3-benzoxazol-2-one Chemical compound C1C(CC2=CC=CC=C12)NC1=NC=C(C=N1)N1CCN(CC1)CC(=O)C1=CC2=C(NC(O2)=O)C=C1 DFGKGUXTPFWHIX-UHFFFAOYSA-N 0.000 description 1
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- OMPJBNCRMGITSC-UHFFFAOYSA-N Benzoylperoxide Chemical compound C=1C=CC=CC=1C(=O)OOC(=O)C1=CC=CC=C1 OMPJBNCRMGITSC-UHFFFAOYSA-N 0.000 description 1
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- VEXZGXHMUGYJMC-UHFFFAOYSA-M Chloride anion Chemical compound [Cl-] VEXZGXHMUGYJMC-UHFFFAOYSA-M 0.000 description 1
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- 238000002848 electrochemical method Methods 0.000 description 1
- 238000003487 electrochemical reaction Methods 0.000 description 1
- 229910052735 hafnium Inorganic materials 0.000 description 1
- VBJZVLUMGGDVMO-UHFFFAOYSA-N hafnium atom Chemical compound [Hf] VBJZVLUMGGDVMO-UHFFFAOYSA-N 0.000 description 1
- 150000008282 halocarbons Chemical class 0.000 description 1
- 150000002391 heterocyclic compounds Chemical class 0.000 description 1
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- 150000002430 hydrocarbons Chemical class 0.000 description 1
- WGCNASOHLSPBMP-UHFFFAOYSA-N hydroxyacetaldehyde Natural products OCC=O WGCNASOHLSPBMP-UHFFFAOYSA-N 0.000 description 1
- 239000011261 inert gas Substances 0.000 description 1
- 229910017053 inorganic salt Inorganic materials 0.000 description 1
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- 238000011068 loading method Methods 0.000 description 1
- 239000011777 magnesium Substances 0.000 description 1
- 229910052749 magnesium Inorganic materials 0.000 description 1
- 229910052748 manganese Inorganic materials 0.000 description 1
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Description
また、このときの攪拌温度は、例えば、10〜30℃、攪拌時間は、例えば、1〜60分間である。
(1) 2H2+4OH−→4H2O+4e− (燃料側電極2における反応)
(2) O2+2H2O+4e−→4OH− (酸素側電極3における反応)
(3) 2H2+O2→2H2O (燃料電池1全体としての反応)
なお、この燃料電池1の運転条件は、特に限定されないが、例えば、燃料側電極2側の加圧が100kPa以下、好ましくは、50kPa以下であり、酸素側電極3側の加圧が100kPa以下、好ましくは、50kPa以下であり、燃料電池セルSの温度が30〜100℃、好ましくは、60〜90℃として設定される。
1)ポリピロールカーボンコンポジット(PPy−C)の作製
純水75mLに、カーボン(E−TEK社製 Vulcan XC−72、比表面積250m2/g)10gと酢酸(酢酸濃度100%)2.5mLとを加え、室温(約25℃)で20分間攪拌して、カーボンが分散したカーボン分散液を調製した。次いで、このカーボン分散液にピロール(Aldrich社製)2gを加え、室温で5分間攪拌した。さらに、このカーボン分散液に濃度10%の過酸化水素10mLを加え、室温で1時間攪拌することにより、ピロールを酸化重合させた。その後、このカーボン分散液を濾過して温水洗浄し、90℃で真空乾燥した。これにより、カーボン上にピロールが重合したPPy−C乾燥粉末を得た。
1)で得られたPPy−C乾燥粉末2gを、純水44mLに加え、80℃まで加熱しながら30分間攪拌して、PPy−Cが分散したPPy−C分散液を得た。次いで、硝酸コバルト(II)六水和物1.1gを、11mLの純水に溶解させ、コバルト含有水溶液を調製した。そして、このコバルト含有水溶液を、PPy−C分散液に加え、80℃で30分間攪拌することによって、コバルト−PPy−C混合液を得た。続いて、水素化ホウ素ナトリウム5.23gと水酸化ナトリウム0.37gとを、500mLの純水に溶解させ、アルカリ水溶液を調製した。次いで、コバルト−PPy−C混合液のpHが11.1になるまで、アルカリ水溶液を徐々に加えた後、このコバルト−PPy−C混合液80℃で30分間放置した。なお、2)におけるこの操作(アルカリ水溶液を加える操作)に至るまでの操作は全て、窒素雰囲気で行なった。その後、コバルト−PPy−C混合液を濾過して温水洗浄し、90℃で真空乾燥した。これにより、PPy−Cにコバルトが担持されたコバルト担持PPy−C(コバルトの担持濃度:10質量%)の乾燥粉末を得た。
コバルト−テトラキス(p−メトキシフェニル)ポルフィリン錯体(CAS No.28903−71−1、アルドリッチ社製)(以下、ポルフィリン錯体と称する。)1gを、テトラヒドロフラン(THF)200mLに溶解させた。
製造例1で得られたコバルト担持PPy−Cの乾燥粉末7mgと、製造例2で得られたポルフィリン錯体の焼成粉末3mgとを混合し(質量比 コバルト担持PPy−C:ポルフィリン錯体=7:3)、混合粉末10mgを得た。
製造例1で得られたコバルト担持PPy−Cの乾燥粉末5mgと、製造例2で得られたポルフィリン錯体の焼成粉末5mgとを混合した(質量比 コバルト担持PPy−C:ポルフィリン錯体=5:5)以外は、参考実施例1と同様にして、テストピース2を得た。
製造例1で得られたコバルト担持PPy−Cの乾燥粉末3mgと、製造例2で得られたポルフィリン錯体の焼成粉末7mgとを混合した(質量比 コバルト担持PPy−C:ポルフィリン錯体=3:7)以外は、参考実施例1と同様にして、テストピース3を得た。
製造例1で得られたコバルト担持PPy−Cの乾燥粉末3mgと、製造例2で得られたポルフィリン錯体の焼成粉末7mgとを混合した(質量比 コバルト担持PPy−C:ポルフィリン錯体=8:2)以外は、参考実施例1と同様にして、テストピース3を得た。
製造例1で得られたコバルト担持PPy−Cの乾燥粉末3mgと、製造例2で得られたポルフィリン錯体の焼成粉末7mgとを混合した(質量比 コバルト担持PPy−C:ポルフィリン錯体=2:8)以外は、参考実施例1と同様にして、テストピース3を得た。
酸素側電極の活性は、回転ディスク電極による電気化学測定法(サイクリックボルタンメトリー)で測定した。
(1)膜−電極接合体の作製
(1−1)燃料側電極の形成
ニッケル0.2gと、2質量%アニオン交換樹脂溶液(溶媒:THF+1−プロパノール(1:4質量比))1.1gとを混合し、得られた混合物を、溶媒(THF+1−プロパノール(1:4質量比))5.1mLに加えた。そして、25℃で15分間撹拌することにより、ニッケルを担持したアニオン交換樹脂の燃料側電極インクを調製した。
製造例1で得られたコバルト担持PPy−Cの乾燥粉末0.1gと、製造例2で得られたポルフィリン錯体の焼成粉末0.1gと(質量比 コバルト担持PPy−C:ポルフィリン錯体=5:5)、2質量%アニオン交換樹脂溶液1.9g(溶媒:THF+1−プロパノール(1:4質量比))とを混合した。
(2)単位セルの組立
(1)で得られた膜−電極接合体の燃料側電極層および空気側電極層それぞれに導電性多孔質体のカーボンシート(ガス拡散層)を接合し、カーボンシートが接合された膜−電極接合体にOリング(シール材)を取り付け、燃料側セパレータと空気側セパレータとで挟み込むことにより、単位セルを組み立てた。
上記(1−2)酸素側電極の形成において、製造例1で得られたコバルト担持PPy−Cの乾燥粉末0.2gを用い、製造例2で得られたポルフィリン錯体の焼成粉末を混合しなかった(質量比 コバルト担持PPy−C:ポルフィリン錯体=10:0)以外は、実施例1(1)と同様にして、膜−電極接合体を作製した。酸素側電極のコバルト担持量は、0.2mg/cm2であった。
上記(1−2)酸素側電極の形成において、製造例1で得られたコバルト担持PPy−Cの乾燥粉末0.18gと、製造例2で得られたポルフィリン錯体の焼成粉末0.02gとを混合した(質量比 コバルト担持PPy−C:ポルフィリン錯体=9:1)以外は、実施例1(1)と同様にして、膜−電極接合体を作製した。酸素側電極のコバルト担持量は、0.2mg/cm2であった。
上記(1−2)酸素側電極の形成において、製造例1で得られたコバルト担持PPy−Cの乾燥粉末0.02gと、製造例2で得られたポルフィリン錯体の焼成粉末0.18gとを混合した(質量比 コバルト担持PPy−C:ポルフィリン錯体=1:9)以外は、実施例1(1)と同様にして、膜−電極接合体を作製した。酸素側電極のコバルト担持量は、0.2mg/cm2であった。
上記(1−2)酸素側電極の形成において、製造例2で得られたポルフィリン錯体の焼成粉末0.2gを用い、製造例1で得られたコバルト担持PPy−Cの乾燥粉末を混合しなかった(質量比 コバルト担持PPy−C:ポルフィリン錯体=0:10)以外は、実施例1(1)と同様にして、膜−電極接合体を作製した。酸素側電極のコバルト担持量は、0.2mg/cm2であった。
実施例1および比較例1〜4で組み立てた単位セルに対して、燃料側電極には水加ヒドラジン1mol/dm3・1N−KOH水溶液を、2mL/minの速度で供給し、空気側電極には、50℃の飽和加湿空気を0.5L/minの速度で供給した。なお、単位セルの運転条件は、供給圧を20kPa・absとし、セル運転温度は80℃とした。
Claims (2)
- アニオン成分を移動させることができる電解質と、前記電解質を挟んで対向配置された燃料側電極および酸素側電極とを含み、
前記酸素側電極は、
ポリピロールとカーボンとからなる複合体、および、前記複合体に担持された第1遷移金属を含む第1触媒と、
ポルフィリン環含有化合物に第2遷移金属が配位されてなるポルフィリン錯体を含む第2触媒と
を含み、
前記第1触媒の配合割合が、前記第1触媒および前記第2触媒の総量100質量部に対して、20〜80質量部であることを特徴とする、燃料電池。 - 前記第1遷移金属および前記第2遷移金属が、コバルトであることを特徴とする、請求項1に記載の燃料電池。
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JP2005044664A (ja) * | 2003-07-23 | 2005-02-17 | Toyota Central Res & Dev Lab Inc | 電極触媒及びその製造方法 |
JP2005066592A (ja) * | 2003-08-05 | 2005-03-17 | Toyota Motor Corp | 触媒材料およびその製造方法 |
WO2006083029A1 (ja) * | 2005-02-03 | 2006-08-10 | Toyota Jidosha Kabushiki Kaisha | 触媒材料およびその製造方法 |
JP2007237092A (ja) * | 2006-03-09 | 2007-09-20 | Toyota Motor Corp | 触媒材料の製造方法 |
WO2008117485A1 (ja) * | 2007-03-27 | 2008-10-02 | Daihatsu Motor Co., Ltd. | 燃料電池 |
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JP2000157871A (ja) * | 1998-11-27 | 2000-06-13 | Japan Science & Technology Corp | 酸素4電子還元触媒 |
JP2005044664A (ja) * | 2003-07-23 | 2005-02-17 | Toyota Central Res & Dev Lab Inc | 電極触媒及びその製造方法 |
JP2005066592A (ja) * | 2003-08-05 | 2005-03-17 | Toyota Motor Corp | 触媒材料およびその製造方法 |
WO2006083029A1 (ja) * | 2005-02-03 | 2006-08-10 | Toyota Jidosha Kabushiki Kaisha | 触媒材料およびその製造方法 |
JP2007237092A (ja) * | 2006-03-09 | 2007-09-20 | Toyota Motor Corp | 触媒材料の製造方法 |
WO2008117485A1 (ja) * | 2007-03-27 | 2008-10-02 | Daihatsu Motor Co., Ltd. | 燃料電池 |
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DE112011101133T5 (de) | 2013-02-07 |
US20130011765A1 (en) | 2013-01-10 |
CN102844921B (zh) | 2015-06-24 |
JPWO2011122399A1 (ja) | 2013-07-08 |
US8945791B2 (en) | 2015-02-03 |
DE112011101133T8 (de) | 2013-04-25 |
CN102844921A (zh) | 2012-12-26 |
WO2011122399A1 (ja) | 2011-10-06 |
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