JP5484120B2 - ガス拡散電極、ガス拡散電極の製造方法、燃料電池および食塩電解セル - Google Patents
ガス拡散電極、ガス拡散電極の製造方法、燃料電池および食塩電解セル Download PDFInfo
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- JP5484120B2 JP5484120B2 JP2010034851A JP2010034851A JP5484120B2 JP 5484120 B2 JP5484120 B2 JP 5484120B2 JP 2010034851 A JP2010034851 A JP 2010034851A JP 2010034851 A JP2010034851 A JP 2010034851A JP 5484120 B2 JP5484120 B2 JP 5484120B2
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- 238000009792 diffusion process Methods 0.000 title claims description 61
- 239000000446 fuel Substances 0.000 title claims description 18
- 238000005868 electrolysis reaction Methods 0.000 title claims description 15
- 238000004519 manufacturing process Methods 0.000 title claims description 15
- 150000003839 salts Chemical class 0.000 title claims description 15
- 239000003054 catalyst Substances 0.000 claims description 88
- 229910052719 titanium Inorganic materials 0.000 claims description 52
- 229910052715 tantalum Inorganic materials 0.000 claims description 40
- 229910052726 zirconium Inorganic materials 0.000 claims description 39
- 229910052758 niobium Inorganic materials 0.000 claims description 36
- 239000000758 substrate Substances 0.000 claims description 36
- 150000004706 metal oxides Chemical class 0.000 claims description 25
- 229910044991 metal oxide Inorganic materials 0.000 claims description 24
- 239000000463 material Substances 0.000 claims description 23
- 229910052751 metal Inorganic materials 0.000 claims description 21
- 239000002184 metal Substances 0.000 claims description 21
- 238000003980 solgel method Methods 0.000 claims description 12
- 239000002131 composite material Substances 0.000 claims description 11
- 150000002500 ions Chemical class 0.000 claims description 10
- 238000003618 dip coating Methods 0.000 claims description 9
- 229910021645 metal ion Inorganic materials 0.000 claims description 9
- 150000002739 metals Chemical class 0.000 claims description 8
- 229910052718 tin Inorganic materials 0.000 claims description 5
- 150000004696 coordination complex Chemical class 0.000 claims description 3
- 239000002905 metal composite material Substances 0.000 claims 1
- 239000010936 titanium Substances 0.000 description 74
- 239000007789 gas Substances 0.000 description 55
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 45
- 239000001301 oxygen Substances 0.000 description 45
- 229910052760 oxygen Inorganic materials 0.000 description 45
- 239000010955 niobium Substances 0.000 description 33
- 239000000243 solution Substances 0.000 description 27
- 239000001257 hydrogen Substances 0.000 description 24
- 229910052739 hydrogen Inorganic materials 0.000 description 24
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 description 24
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 22
- 239000012702 metal oxide precursor Substances 0.000 description 22
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 description 18
- 238000006722 reduction reaction Methods 0.000 description 17
- 239000002245 particle Substances 0.000 description 14
- 239000003014 ion exchange membrane Substances 0.000 description 10
- 229910052697 platinum Inorganic materials 0.000 description 10
- 238000006243 chemical reaction Methods 0.000 description 9
- 238000000034 method Methods 0.000 description 9
- XOLBLPGZBRYERU-UHFFFAOYSA-N tin dioxide Chemical compound O=[Sn]=O XOLBLPGZBRYERU-UHFFFAOYSA-N 0.000 description 9
- 150000001875 compounds Chemical class 0.000 description 8
- 239000012528 membrane Substances 0.000 description 8
- 229910001887 tin oxide Inorganic materials 0.000 description 8
- OGIDPMRJRNCKJF-UHFFFAOYSA-N titanium oxide Inorganic materials [Ti]=O OGIDPMRJRNCKJF-UHFFFAOYSA-N 0.000 description 8
- 238000010304 firing Methods 0.000 description 7
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 description 6
- 230000003197 catalytic effect Effects 0.000 description 6
- 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 description 6
- 229910001924 platinum group oxide Inorganic materials 0.000 description 6
- 239000002904 solvent Substances 0.000 description 6
- GUVRBAGPIYLISA-UHFFFAOYSA-N tantalum atom Chemical compound [Ta] GUVRBAGPIYLISA-UHFFFAOYSA-N 0.000 description 6
- 229910001936 tantalum oxide Inorganic materials 0.000 description 6
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 description 5
- 239000010419 fine particle Substances 0.000 description 5
- 239000000047 product Substances 0.000 description 5
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 5
- 230000010757 Reduction Activity Effects 0.000 description 4
- QCWXUUIWCKQGHC-UHFFFAOYSA-N Zirconium Chemical compound [Zr] QCWXUUIWCKQGHC-UHFFFAOYSA-N 0.000 description 4
- 238000005341 cation exchange Methods 0.000 description 4
- HTXDPTMKBJXEOW-UHFFFAOYSA-N dioxoiridium Chemical compound O=[Ir]=O HTXDPTMKBJXEOW-UHFFFAOYSA-N 0.000 description 4
- 238000001035 drying Methods 0.000 description 4
- 229910000457 iridium oxide Inorganic materials 0.000 description 4
- 239000000203 mixture Substances 0.000 description 4
- 230000003647 oxidation Effects 0.000 description 4
- 238000007254 oxidation reaction Methods 0.000 description 4
- RVTZCBVAJQQJTK-UHFFFAOYSA-N oxygen(2-);zirconium(4+) Chemical compound [O-2].[O-2].[Zr+4] RVTZCBVAJQQJTK-UHFFFAOYSA-N 0.000 description 4
- -1 tin alkoxides Chemical class 0.000 description 4
- 229910001928 zirconium oxide Inorganic materials 0.000 description 4
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 3
- LYCAIKOWRPUZTN-UHFFFAOYSA-N Ethylene glycol Chemical compound OCCO LYCAIKOWRPUZTN-UHFFFAOYSA-N 0.000 description 3
- 239000006229 carbon black Substances 0.000 description 3
- KRKNYBCHXYNGOX-UHFFFAOYSA-N citric acid Chemical compound OC(=O)CC(O)(C(O)=O)CC(O)=O KRKNYBCHXYNGOX-UHFFFAOYSA-N 0.000 description 3
- 238000000576 coating method Methods 0.000 description 3
- 238000002484 cyclic voltammetry Methods 0.000 description 3
- 239000003792 electrolyte Substances 0.000 description 3
- 230000002209 hydrophobic effect Effects 0.000 description 3
- 229910052741 iridium Inorganic materials 0.000 description 3
- GKOZUEZYRPOHIO-UHFFFAOYSA-N iridium atom Chemical compound [Ir] GKOZUEZYRPOHIO-UHFFFAOYSA-N 0.000 description 3
- 229920000642 polymer Polymers 0.000 description 3
- 239000007784 solid electrolyte Substances 0.000 description 3
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 2
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 description 2
- MYMOFIZGZYHOMD-UHFFFAOYSA-N Dioxygen Chemical compound O=O MYMOFIZGZYHOMD-UHFFFAOYSA-N 0.000 description 2
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 2
- LRHPLDYGYMQRHN-UHFFFAOYSA-N N-Butanol Chemical compound CCCCO LRHPLDYGYMQRHN-UHFFFAOYSA-N 0.000 description 2
- QAOWNCQODCNURD-UHFFFAOYSA-N Sulfuric acid Chemical compound OS(O)(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-N 0.000 description 2
- 229910052787 antimony Inorganic materials 0.000 description 2
- WATWJIUSRGPENY-UHFFFAOYSA-N antimony atom Chemical compound [Sb] WATWJIUSRGPENY-UHFFFAOYSA-N 0.000 description 2
- 239000011230 binding agent Substances 0.000 description 2
- 238000001354 calcination Methods 0.000 description 2
- 229910052799 carbon Inorganic materials 0.000 description 2
- 239000003575 carbonaceous material Substances 0.000 description 2
- 239000011248 coating agent Substances 0.000 description 2
- 229910001882 dioxygen Inorganic materials 0.000 description 2
- 238000011156 evaluation Methods 0.000 description 2
- 150000002431 hydrogen Chemical class 0.000 description 2
- 239000011259 mixed solution Substances 0.000 description 2
- 150000002823 nitrates Chemical class 0.000 description 2
- 229910003446 platinum oxide Inorganic materials 0.000 description 2
- 229910001925 ruthenium oxide Inorganic materials 0.000 description 2
- WOCIAKWEIIZHES-UHFFFAOYSA-N ruthenium(iv) oxide Chemical compound O=[Ru]=O WOCIAKWEIIZHES-UHFFFAOYSA-N 0.000 description 2
- 229920006395 saturated elastomer Polymers 0.000 description 2
- 239000007787 solid Substances 0.000 description 2
- 230000003068 static effect Effects 0.000 description 2
- 239000000126 substance Substances 0.000 description 2
- PYKSLEHEVAWOTJ-UHFFFAOYSA-N tetrabutoxystannane Chemical compound CCCCO[Sn](OCCCC)(OCCCC)OCCCC PYKSLEHEVAWOTJ-UHFFFAOYSA-N 0.000 description 2
- 238000005979 thermal decomposition reaction Methods 0.000 description 2
- 239000011882 ultra-fine particle Substances 0.000 description 2
- 229920003934 Aciplex® Polymers 0.000 description 1
- 239000004215 Carbon black (E152) Substances 0.000 description 1
- VEXZGXHMUGYJMC-UHFFFAOYSA-M Chloride anion Chemical compound [Cl-] VEXZGXHMUGYJMC-UHFFFAOYSA-M 0.000 description 1
- 229910001111 Fine metal Inorganic materials 0.000 description 1
- 229920003935 Flemion® Polymers 0.000 description 1
- 229920000557 Nafion® Polymers 0.000 description 1
- KJTLSVCANCCWHF-UHFFFAOYSA-N Ruthenium Chemical compound [Ru] KJTLSVCANCCWHF-UHFFFAOYSA-N 0.000 description 1
- 229910006404 SnO 2 Inorganic materials 0.000 description 1
- JHGFRCLDPHKRBS-UHFFFAOYSA-N [Sn+2]=O.[O-2].[Zr+4].[O-2].[O-2] Chemical compound [Sn+2]=O.[O-2].[Zr+4].[O-2].[O-2] JHGFRCLDPHKRBS-UHFFFAOYSA-N 0.000 description 1
- 239000002253 acid Substances 0.000 description 1
- 230000002378 acidificating effect Effects 0.000 description 1
- 239000007864 aqueous solution Substances 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- PVZMSIQWTGPSHJ-UHFFFAOYSA-N butan-1-ol;tantalum Chemical compound [Ta].CCCCO.CCCCO.CCCCO.CCCCO.CCCCO PVZMSIQWTGPSHJ-UHFFFAOYSA-N 0.000 description 1
- 239000001569 carbon dioxide Substances 0.000 description 1
- 229910002092 carbon dioxide Inorganic materials 0.000 description 1
- 150000004649 carbonic acid derivatives Chemical class 0.000 description 1
- 150000001805 chlorine compounds Chemical class 0.000 description 1
- 238000000975 co-precipitation Methods 0.000 description 1
- 238000005260 corrosion Methods 0.000 description 1
- 230000007797 corrosion Effects 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- 238000004090 dissolution Methods 0.000 description 1
- UQSQSQZYBQSBJZ-UHFFFAOYSA-N fluorosulfonic acid Chemical compound OS(F)(=O)=O UQSQSQZYBQSBJZ-UHFFFAOYSA-N 0.000 description 1
- 238000009689 gas atomisation Methods 0.000 description 1
- 239000002815 homogeneous catalyst Substances 0.000 description 1
- 229930195733 hydrocarbon Natural products 0.000 description 1
- 150000002430 hydrocarbons Chemical class 0.000 description 1
- QWPPOHNGKGFGJK-UHFFFAOYSA-N hypochlorous acid Chemical compound ClO QWPPOHNGKGFGJK-UHFFFAOYSA-N 0.000 description 1
- 229920000554 ionomer Polymers 0.000 description 1
- 239000007769 metal material Substances 0.000 description 1
- GUCVJGMIXFAOAE-UHFFFAOYSA-N niobium atom Chemical compound [Nb] GUCVJGMIXFAOAE-UHFFFAOYSA-N 0.000 description 1
- 229910052757 nitrogen Inorganic materials 0.000 description 1
- 229910000510 noble metal Inorganic materials 0.000 description 1
- 239000011368 organic material Substances 0.000 description 1
- 238000005192 partition Methods 0.000 description 1
- 230000002093 peripheral effect Effects 0.000 description 1
- 239000004033 plastic Substances 0.000 description 1
- 239000005518 polymer electrolyte Substances 0.000 description 1
- 229920006254 polymer film Polymers 0.000 description 1
- 238000006116 polymerization reaction Methods 0.000 description 1
- 239000011148 porous material Substances 0.000 description 1
- 239000002244 precipitate Substances 0.000 description 1
- 239000002994 raw material Substances 0.000 description 1
- 230000009257 reactivity Effects 0.000 description 1
- 229910052707 ruthenium Inorganic materials 0.000 description 1
- VSZWPYCFIRKVQL-UHFFFAOYSA-N selanylidenegallium;selenium Chemical compound [Se].[Se]=[Ga].[Se]=[Ga] VSZWPYCFIRKVQL-UHFFFAOYSA-N 0.000 description 1
- 239000007921 spray Substances 0.000 description 1
- 150000003467 sulfuric acid derivatives Chemical class 0.000 description 1
- 238000003786 synthesis reaction Methods 0.000 description 1
- QHGNHLZPVBIIPX-UHFFFAOYSA-N tin(ii) oxide Chemical compound [Sn]=O QHGNHLZPVBIIPX-UHFFFAOYSA-N 0.000 description 1
- 229910052845 zircon Inorganic materials 0.000 description 1
- GFQYVLUOOAAOGM-UHFFFAOYSA-N zirconium(iv) silicate Chemical compound [Zr+4].[O-][Si]([O-])([O-])[O-] GFQYVLUOOAAOGM-UHFFFAOYSA-N 0.000 description 1
Classifications
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/30—Hydrogen technology
- Y02E60/50—Fuel cells
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
- Y02P70/50—Manufacturing or production processes characterised by the final manufactured product
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- Inert Electrodes (AREA)
- Fuel Cell (AREA)
- Catalysts (AREA)
- Electrodes For Compound Or Non-Metal Manufacture (AREA)
- Chemically Coating (AREA)
Description
図1(a)、(b)、(c)は、本発明を適用したガス拡散電極の断面構成を示す説明図、基材として用いたTi焼結体を電子顕微鏡で観察したときの説明図、およびTi焼結体の表面に触媒層を形成した様子を顕微鏡で観察したときの説明図である。図2は、本発明を適用したガス拡散電極の製造方法を示す説明図である。
上記の触媒層の製造方法において、金属酸化物前駆体溶液を調製する際に、Snのイオンを含む化合物を添加してもよい(図2のカッコ書き参照)。
図3(a)、(b)は各々、本発明を適用したガス拡散電極を用いた燃料電池および食塩電解用の電解セルの説明図である。本発明を適用したガス拡散電極は、以下に説明するように燃料電池および食塩電解用の電解セルに用いられる。
図3(a)は、本発明のガス拡散電極を使用した燃料電池を例示する概略断面図である。イオン交換膜燃料電池においては、イオン交換膜の特性が重要であるが、イオン交換膜として化学的安定性に優れたものには、ポリパーフルオロスルホン酸を成膜したものが知られており、例えば、米国デュポン社製:商品名ナフィオン、旭硝子(株)製:商品名フレミオン、旭化成ケミカルズ(株)製:商品名アシプレックス等がある。最近では、酸化耐性の優れた膜、PBIなどの炭化水素系膜でも高耐食性、メタノールなどの有機原料の透過防止性に優れた市販品もあり、利用可能である。
図3(b)は、本発明のガス拡散電極をガス拡散陰極に使用した食塩電解用の3室法電解セルを例示する概略断面図である。図3(b)に示す3室法電解セル21は、パーフルオロスルホン酸系の陽イオン交換膜22により、陽極室23と陰極室24と区画されている。陽イオン交換膜22の陽極室23側には、多孔性の陽極25が密着し、陽イオン交換膜22の陰極室側には間隔を空けて、ガス拡散陰極26が設置されている。かかるガス拡散陰極26によって、陰極室24は、陽イオン交換膜22側の陰極液室27と反対側の陰極ガス室28とに区画されている。
2HO2 + 2e → 2OH-+ H2(-0.83V)
に代えて、陰極で以下の反応
2O2 + 2H2 + 4e → 4OH-(0.40V)
を行なわせる。このため、理論的には1.23V、実用的電流密度範囲でも0.8V程度の槽電圧を低減することができ、省電力化を図ることができる。
Claims (9)
- 基材と、
前記基材の表面に形成された触媒層とを有し、
前記基材は、Tiからなり、
前記触媒層の主成分は、Zr、Ti、NbおよびTaから選ばれた1種の金属の酸化物、または、Zr、Ti、NbおよびTaから選ばれた2種以上の金属の複合酸化物からなることを特徴とするガス拡散電極。 - 前記基材は、多孔性基材であることを特徴とする請求項1に記載のガス拡散電極。
- 前記基材は、繊維状の多孔性基材または焼結体からなる多孔性基材であることを特徴とする請求項2に記載のガス拡散電極。
- 前記触媒層の成分として、Snの酸化物が添加されていることを特徴とする請求項1乃至3の何れか一項に記載のガス拡散電極。
- 基材の表面に触媒層が形成されたガス拡散電極の製造方法において、
Tiからなる前記基材を用い、
Zr、Ti、NbおよびTaから選ばれた1種以上の金属のイオンを含む溶液を用い、ゾルゲル法により、前記基材の表面に前記金属の酸化物または前記金属の複合酸化物を前記触媒層として形成することを特徴とするガス拡散電極の製造方法。 - Zr、Ti、NbおよびTaから選ばれた1種以上の金属のイオン並びにSnのイオンを含む溶液を用い、ゾルゲル法により、前記基材の表面に前記金属の酸化物または前記金属の複合酸化物を前記触媒層として形成することを特徴とする請求項5に記載のガス拡散電極の製造方法。
- 前記ゾルゲル法として、ディップコート法を用いることを特徴とする請求項5または6に記載のガス拡散電極の製造方法。
- 請求項1乃至4の何れか一項に記載のガス拡散電極を備えていることを特徴とする燃料電池。
- 請求項1乃至4の何れか一項に記載のガス拡散電極を備えていることを特徴とする食塩電解セル。
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