JP5660879B2 - カソード側触媒層、膜電極接合体、固体高分子型燃料電池及びその製造方法 - Google Patents
カソード側触媒層、膜電極接合体、固体高分子型燃料電池及びその製造方法 Download PDFInfo
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- 239000003054 catalyst Substances 0.000 title claims description 198
- 239000000446 fuel Substances 0.000 title claims description 73
- 239000012528 membrane Substances 0.000 title claims description 40
- 239000005518 polymer electrolyte Substances 0.000 title claims description 18
- 238000004519 manufacturing process Methods 0.000 title claims description 13
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical group [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 claims description 196
- 229910052697 platinum Inorganic materials 0.000 claims description 98
- 239000001301 oxygen Substances 0.000 claims description 82
- 229910052760 oxygen Inorganic materials 0.000 claims description 82
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims description 81
- 238000009792 diffusion process Methods 0.000 claims description 68
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- 229910052748 manganese Inorganic materials 0.000 description 1
- 239000011572 manganese Substances 0.000 description 1
- 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 description 1
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- 229910052762 osmium Inorganic materials 0.000 description 1
- SYQBFIAQOQZEGI-UHFFFAOYSA-N osmium atom Chemical compound [Os] SYQBFIAQOQZEGI-UHFFFAOYSA-N 0.000 description 1
- 150000002926 oxygen Chemical class 0.000 description 1
- 229910052763 palladium Inorganic materials 0.000 description 1
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- MHOVAHRLVXNVSD-UHFFFAOYSA-N rhodium atom Chemical compound [Rh] MHOVAHRLVXNVSD-UHFFFAOYSA-N 0.000 description 1
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Description
[形態1] 電解質膜を有する固体高分子型燃料電池に用いられるカソード側触媒層であって、
前記電解質膜に近接する前記カソード側触媒層の反応面における1cm 2 あたりの重量が0.2mgよりも大きく且つ0.3mg以下である触媒と、
温度80℃及び相対湿度50%の環境下において2.2×10 -14 mol/m/s/Pa以上の酸素透過性を有する電解質樹脂と、
を備え、
前記触媒は、前記反応面の1cm 2 あたり200cm 2 以下の表面積を有する、カソード側触媒層。
前記電解質膜に近接する前記カソード側触媒層の反応面における1cm2あたりの重量が0.3mg以下である触媒と、
温度80℃及び相対湿度50%の環境下において2.2×10-14mol/m/s/Pa以上の酸素透過性を有する電解質樹脂と、
を備える、カソード側触媒層。
前記触媒は、前記反応面における1cm2あたりの重量が0.1mg以下である、カソード側触媒層。
前記触媒は、前記反応面の1cm2あたり200cm2以下の表面積を有する、カソード側触媒層。
前記触媒は、白金である、カソード側触媒層。
温度80℃及び相対湿度50%の環境下において2.2×10-14mol/m/s/Pa以上の酸素透過性を有する電解質樹脂と、酸素還元反応用の触媒とからなるカソード側触媒層であって、反応面における1cm2あたりの前記触媒の重量が0.3mg以下であるカソード側触媒層を、電解質膜上又はガス拡散層用部材上に形成する工程を備える、製造方法。
A1.燃料電池の構成:
図1は、本発明の一実施形態としての触媒層を適用した燃料電池を示す断面図である。燃料電池10は、固体高分子型燃料電池であり、燃料ガスと酸化剤ガスとを用いた電気化学反応により発電を行う。本実施例において、燃料ガスは水素ガスであり、酸化剤ガスは空気である。燃料電池10は、例えば、電気自動車の駆動用電源を供給するための燃料電池スタックに用いられる。燃料電池10は、電解質膜30と、カソード側触媒層31cと、カソード側ガス拡散層32cと、カソード側セパレータ33cと、アノード側触媒層31aと、アノード側ガス拡散層32aと、アノード側セパレータ33aとを備えている。
図3は、カソード側触媒層の白金目付け量と燃料電池10の発電効率(性能)と関係を示す説明図である。図3において、横軸は電流密度(A/cm2)を示し、縦軸はセル電圧(V)を示す。また、図3において、太い実線で示す曲線L1は、白金目付け量が多い場合(例えば、0.5mg/cm2)における燃料電池性能(電流密度に対するセル電圧)のシミュレーション結果を示す。また、細い実線で示す曲線L2は、白金目付け量が少ない場合(例えば、0.2mg/cm2)における燃料電池性能のシミュレーション結果を示す。また、破線で示す曲線L3は、後述するMEAの反応面積あたりの触媒活性の低下分に相当する電圧のシミュレーション結果を示す。
図8は、本実施例のアイオノマーの酸素透過性を示す説明図である。図8において、横軸は相対湿度を、縦軸は酸素透過性(mol/m/s/Pa)すなわち、[mol/(m・s・Pa)]を示す。また図8では、本実施例のアイオノマー(以下、「第1アイオノマー」とも呼ぶ)の酸素透過性を実線で、比較例としての従来のアイオノマー(以下、「第2アイオノマー」とも呼ぶ)の酸素透過性を破線で、それぞれ示す。第1アイオノマー及び第2アイオノマーの酸素透過性の測定は、各アイオノマーを薄い(厚さ0.2ミリメートル程度の)膜状にキャスト成型し、マイクロPt電極を用いたポテンシャルステップ法(ECS Transaction, 16(2),881-889(2008)参照)を用いて行った。
なお、上記各実施例における構成要素の中の、独立クレームでクレームされた要素以外の要素は、付加的な要素であり、適宜省略可能である。また、この発明は上記の実施例や実施形態に限られるものではなく、その要旨を逸脱しない範囲において種々の態様において実施することが可能であり、例えば次のような変形も可能である。
上記実施形態及び実施例では、触媒(触媒粒子120)として白金が用いられていたが、本発明はこれに限定されるものではない。触媒材料としては、金、銀、ルテニウム、ロジウム、パラジウム、オスミウム、イリジウム等の貴金属や、鉄、ニッケル、マンガン、コバルト、クロム、銅、亜鉛、モリブデン、タングステン、ゲルマニウム、錫等の卑金属や、これら貴金属と卑金属との合金、また金属酸化物、金属錯体などの化合物を採用することもできる。すなわち、一般には、上記式(1)に示す酸素還元反応用の任意の触媒を、本発明の触媒層に採用することができる。
上記実施形態及び実施例では、カソード側触媒層31cの形成方法として、電解質膜30又はカソード側ガス拡散層32cに触媒層用スラリーを塗布する方法を採用していたが、本発明はこれに限定されるものではない。触媒担持カーボン110とアイオノマー140とを含む複合粉体をスプレードライ法により製造し、得られた複合粉体を静電スクリーン法等により燃料電池10又はカソード側ガス拡散層32c上に堆積させることによりカソード側触媒層31cを形成することもできる。
上記実施形態では、燃料電池10は、電気自動車の駆動用電源を供給するための燃料電池スタックに用いられていたが、これに代えて、ハイブリッド自動車,船舶,ロボットなどの各種移動体用の燃料電池スタックや、ビルや一般住宅等の建物における定置型電源用の燃料電池スタックに用いることもできる。
20…膜電極接合体(MEA)
30…電解質膜
31a…アノード側触媒層
31c…カソード側触媒層
32a…アノード側ガス拡散層
32c…カソード側ガス拡散層
33a…アノード側セパレータ
33c…カソード側セパレータ
34a…燃料ガス流路
34c…酸化剤ガス流路
110…触媒担持カーボン
120…触媒粒子
130…カーボン担体
140…アイオノマー
145…酸素供給アイオノマー
150…酸素非供給アイオノマー
Claims (6)
- 電解質膜を有する固体高分子型燃料電池に用いられるカソード側触媒層であって、
前記電解質膜に近接する前記カソード側触媒層の反応面における1cm2あたりの重量が0.2mgよりも大きく且つ0.3mg以下である触媒と、
温度80℃及び相対湿度50%の環境下において2.2×10-14mol/m/s/Pa以上の酸素透過性を有する電解質樹脂と、
を備え、
前記触媒は、前記反応面の1cm 2 あたり200cm 2 以下の表面積を有する、カソード側触媒層。 - 請求項1に記載のカソード側触媒層であって、
前記触媒は、前記反応面における1cm2あたりの重量が0.1mg以下である、カソード側触媒層。 - 請求項1または請求項2に記載のカソード側触媒層において、
前記触媒は、白金である、カソード側触媒層。 - 請求項1から請求項3のいずれか一項に記載のカソード側触媒層を備える、膜電極接合体。
- 請求項1から請求項4のいずれか一項に記載のカソード側触媒層を備える、固体高分子型燃料電池。
- 固体高分子型燃料電池の製造方法であって、
温度80℃及び相対湿度50%の環境下において2.2×10-14mol/m/s/Pa以上の酸素透過性を有する電解質樹脂と、酸素還元反応用の触媒とからなるカソード側触媒層であって、反応面における1cm2あたりの前記触媒の重量が0.2mgよりも大きく且つ0.3mg以下であるカソード側触媒層を、電解質膜上又はガス拡散層用部材上に形成する工程を備え、
前記触媒は、前記反応面の1cm 2 あたり200cm 2 以下の表面積を有する、製造方法。
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