JP2018517239A - 燃料電池において過電圧を求める方法 - Google Patents
燃料電池において過電圧を求める方法 Download PDFInfo
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- 239000000446 fuel Substances 0.000 title claims abstract description 60
- 238000000034 method Methods 0.000 title claims abstract description 21
- 239000012528 membrane Substances 0.000 claims abstract description 52
- 239000003792 electrolyte Substances 0.000 claims abstract description 18
- 229910052739 hydrogen Inorganic materials 0.000 claims abstract description 16
- 239000001257 hydrogen Substances 0.000 claims abstract description 16
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 claims abstract description 12
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 claims abstract description 11
- 239000003054 catalyst Substances 0.000 claims abstract description 10
- 239000005518 polymer electrolyte Substances 0.000 claims abstract description 10
- 238000005259 measurement Methods 0.000 claims abstract description 6
- 238000003487 electrochemical reaction Methods 0.000 claims abstract description 5
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 11
- 229910052760 oxygen Inorganic materials 0.000 description 11
- 239000001301 oxygen Substances 0.000 description 11
- 238000013461 design Methods 0.000 description 6
- 238000006243 chemical reaction Methods 0.000 description 5
- 238000006722 reduction reaction Methods 0.000 description 5
- 238000007254 oxidation reaction Methods 0.000 description 4
- 239000003570 air Substances 0.000 description 3
- 230000008901 benefit Effects 0.000 description 3
- 230000007423 decrease Effects 0.000 description 3
- 238000004088 simulation Methods 0.000 description 3
- 239000007787 solid Substances 0.000 description 3
- 230000009471 action Effects 0.000 description 2
- 230000005540 biological transmission Effects 0.000 description 2
- 238000004364 calculation method Methods 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- 125000004435 hydrogen atom Chemical group [H]* 0.000 description 2
- 239000002184 metal Substances 0.000 description 2
- 230000036647 reaction Effects 0.000 description 2
- 230000002441 reversible effect Effects 0.000 description 2
- 238000000926 separation method Methods 0.000 description 2
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 1
- -1 HOR hydrogen Chemical class 0.000 description 1
- 230000004913 activation Effects 0.000 description 1
- 238000013459 approach Methods 0.000 description 1
- 229910052799 carbon Inorganic materials 0.000 description 1
- 230000008859 change Effects 0.000 description 1
- 239000002800 charge carrier Substances 0.000 description 1
- 230000003247 decreasing effect Effects 0.000 description 1
- 230000005611 electricity Effects 0.000 description 1
- 238000000157 electrochemical-induced impedance spectroscopy Methods 0.000 description 1
- 238000004070 electrodeposition Methods 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 150000002431 hydrogen Chemical class 0.000 description 1
- 238000001566 impedance spectroscopy Methods 0.000 description 1
- 238000000608 laser ablation Methods 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 238000012821 model calculation Methods 0.000 description 1
- 239000007800 oxidant agent Substances 0.000 description 1
- 230000001590 oxidative effect Effects 0.000 description 1
- 238000010248 power generation Methods 0.000 description 1
- 230000008569 process Effects 0.000 description 1
- 239000000376 reactant Substances 0.000 description 1
- 238000012360 testing method Methods 0.000 description 1
- 239000011800 void material Substances 0.000 description 1
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Abstract
【数1】
この際、σm=電解質膜のイオン伝導性(Ω−1cm−1)、bw=作用電極の電気化学的反応のための半電池のターフェル勾配、Im=膜層厚(cm)及びjw 0=電極単位表面積当たりの作用電極の触媒の交換電流密度(Acm−2)。この配置を用いることによって、水素が供給された参照電極のところで測定された電位が、十分な精度で、作用電極の過電圧に相当することを有利に保証できる。この方法は、ポリマー−電解質膜燃料電池(PEM−FC)、直接メタノール燃料電池(DMFC)にまたは高温燃料電池(SOFC)にも、使用可能である。
Description
〜は無次元の変数を示す。
b アノードもしくはカソード反応のための半電池のターフェル勾配(V)
Eeq 半電池の平衡電位(V)
F ファラデー定数
J 作用領域中の平均電流密度(Acm−2)
ja アノード側上での局所的プロトン−電流密度(Acm−2)
jc カソード側上での局所的プロトン−電流密度(Acm−2)
jhy 水素交換電流密度(Acm−2)
jhy 0 作用領域中での水素交換電流密度(Acm−2)
jox 酸素交換電流密度(Acm−2)
jox 0 作用領域中での酸素交換電流密度(Acm−2)
Lgap 対電極の縁と参照電極の縁との間の最小間隔
Ll,x 対電極の直線状縁とηc +=boxである点との間の間隔(cm)
L1,r 対電極の縁とηc +=boxである点との間の半径間隔(cm)
lm 膜層厚(cm)
r 半径位置
Ra アノード半径
Rc カソード半径
z 膜表面に対して垂直な座標(cm)
この際、以下の下付の添え字が使用される:
a アノード
c カソード
HOR 水素酸化反応(英語 hydrogen oxidation reaction)
hy 水素
m 膜
ORR 酸素還元反応(英語 oxygen reduction reaction)
ox 酸素
ref 参照電極
x 対電極(counter electrode)の直線状の縁を持つシステム
更に、以下の上付きの添え字が使用される:
+ 正側値
加えて、以下にリストするギリシア文字が使用される:
η 局所的過電圧(V)
ηc +,0 r=0での正側カソード過電圧(V)
σm 膜のイオン伝導性(Ω−1cm−1)
Φ 膜電位(V)
Φ+ 正側膜電位(V)
Φ+,∞ γ→∞の場合の正側膜電位(V)
φ 炭素相の電位(V)
図6に示す様に形状及び座標系を有する同心的な電極を備えたPEM−FCを考察する。層厚lmを有するポリマー電解質膜の両側に、電極として大表面積のカソード並びに小さなアノードが配置されている。電極と膜との間には、通常、(図7には図示されていない)然るべき触媒層、特にアノード触媒層(ACL=anode catalyst layer)並びにカソード触媒層(CCL=cathode catalyst layer)が存在する。
図7では、様々なアノード半径Raについての方程式14の解を示す。この問題の特別な特徴は、アノード縁の非常に近くで、酸素還元反応(ORR)の電位ηc +の勾配が、アノード半径が小さくなるほど大きくなることである。これは、荷電した金属先端と平面との間のラプラス電位の挙動と質的に類似し;金属先端の半径が狭くなるほど、先端付近の電位が軸対称性に依存して大きく減少する。
Claims (10)
- ポリマー−電解質膜を含む燃料電池における作用電極の過電圧を求める方法において、前記ポリマー−電解質膜の一方の面には連続的な作用電極を、そして他方の面には対電極が配置されており、かつ接地された対電極に対する参照電極の電位が測定される方法であって、
−前記測定のために、対電極が少なくとも一つの側縁を有しかつこの縁の少なくとも一つの領域において、局所的半径Raを有する凸状湾曲を有すること、
−対電極に隣接しかつ作用電極とは反対側の電解質膜表面が、電極不在領域を有すること、
−参照電極が、電解質膜表面上で、電極不在領域の範囲内にかつ対電極の凸状縁領域の直近に、間隔Lgapで配置されていること、
−この際、上記範囲中の参照電極と対電極の凸状に湾曲した縁領域との間のLgapの最小間隔が以下によって与えられること、
を特徴とする前記方法。
σm=電解質膜のイオン伝導性(Ω−1cm−1)、
box=作用電極の電気化学的反応のための半電池のターフェル勾配(V)、
lm=膜層厚(cm)、
jox 0=電極単位面積当たりの作用電極の触媒の交換電流密度(Acm−2)、及び
Ra=対電極の凸状に湾曲した縁領域の半径(cm)。 - 参照電極と対電極の凸状に湾曲した縁領域との間の間隔が、対電極の凸状に湾曲した縁領域からLgap〜100Lgapの範囲、有利にはLgap〜10Lgapとの間の範囲、特に有利にはLgap〜3Lgapとの間の範囲で選択される、請求項1に記載の方法。
- 該方法の間に参照電極に水素が供給される、請求項1または2に記載の方法。
- 対電極としてはアノードが、及び作用電極としてはカソードが使用される、請求項1〜3のいずれか一つに記載の方法。
- 対電極の湾曲した縁領域の局所的曲率半径として、0.01と1cmとの間の値、特に0.1cm未満の値が選択される、請求項1〜4のいずれか一つに記載の方法。
- ポリマー−電解質膜燃料電池(PEM−FC)、直接メタノール燃料電池(DMFC)または高温燃料電池(SOFCまたはHT−PEM−FC)が燃料電池として使用される、請求項1〜5のいずれか一つに記載の方法。
- 請求項1〜6のいずれか一つに記載の方法を実施するための燃料電池装置であって、
− 一方の面上には連続的な作用電極が、他方の面上には対電極が配置されている、層厚lmを有するポリマー電解質膜を含み、
− この際、前記対電極は、少なくとも一つの側縁を有し、及びこの縁の少なくとも一つの領域に、局所的半径Raを有する凸状湾曲を有し、
− この際、対電極に隣接しかつ作用電極とは反対側の電解質膜表面が、電極不在領域を有し、
− この際、参照電極が、電解質膜表面上で、電極不在領域の範囲内にかつ対電極の凸状縁領域の直近に配置され、
− この際、参照電極と対電極の凸状に湾曲した縁領域との間の最小間隔Lgapが以下によって与えられ、
σm=電解質膜のイオン伝導性(Ω−1cm−1)、
box=作用電極の電気化学的反応のための半電池のターフェル勾配(V)、
lm=膜層厚(cm)、
jox 0=電極単位面積当たりの作用電極の触媒の交換電流密度(Acm−2)、及び
Ra=参照電極に最も近い、対電極の凸状に湾曲した縁領域の局所的半径(cm)、及び
− この際、参照電極が、対電極の凸状に湾曲した縁領域からLgap〜100Lgapの範囲、有利にはLgap〜10Lgapとの間の範囲、特にLgap〜3Lgapの範囲の間隔で配置されている、
前記燃料電池装置。 - 作用電極としてカソードを及び対電極としてアノードを備える、請求項7に記載の燃料電池装置。
- 凸状に湾曲した縁領域が、0.01と1cmとの間、特に0.1cm未満の局所的半径Raを有する、請求項7〜8のいずれか一つに記載の燃料電池装置。
- 連続的な作用電極の寸法が3λD超である、請求項7〜9のいずれか一つに記載の燃料電池装置。
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JP2006351404A (ja) * | 2005-06-17 | 2006-12-28 | Nippon Telegr & Teleph Corp <Ntt> | 電極過電圧分離測定用の参照極を設けた燃料電池セルおよびその製造方法 |
WO2007110970A1 (ja) * | 2006-03-29 | 2007-10-04 | The Tokyo Electric Power Company, Incorporated | 界面抵抗の算出方法 |
JP2010061887A (ja) * | 2008-09-02 | 2010-03-18 | Yokogawa Electric Corp | 燃料電池用の電極触媒の性能評価方法および評価装置 |
JP2011040362A (ja) * | 2009-07-14 | 2011-02-24 | Kansai Electric Power Co Inc:The | 固体酸化物形燃料電池用燃料極、固体酸化物形燃料電池および固体酸化物形燃料電池の作動方法 |
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JP2006351404A (ja) * | 2005-06-17 | 2006-12-28 | Nippon Telegr & Teleph Corp <Ntt> | 電極過電圧分離測定用の参照極を設けた燃料電池セルおよびその製造方法 |
WO2007110970A1 (ja) * | 2006-03-29 | 2007-10-04 | The Tokyo Electric Power Company, Incorporated | 界面抵抗の算出方法 |
JP2010061887A (ja) * | 2008-09-02 | 2010-03-18 | Yokogawa Electric Corp | 燃料電池用の電極触媒の性能評価方法および評価装置 |
JP2011040362A (ja) * | 2009-07-14 | 2011-02-24 | Kansai Electric Power Co Inc:The | 固体酸化物形燃料電池用燃料極、固体酸化物形燃料電池および固体酸化物形燃料電池の作動方法 |
JP2013114931A (ja) * | 2011-11-29 | 2013-06-10 | Honda Motor Co Ltd | 固体高分子型燃料電池用電解質膜・電極構造体 |
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US11024862B2 (en) | 2021-06-01 |
DE102015005220A1 (de) | 2016-10-27 |
JP6732793B2 (ja) | 2020-07-29 |
CN107534173B (zh) | 2020-12-01 |
US10637083B2 (en) | 2020-04-28 |
EP3286793A1 (de) | 2018-02-28 |
CN107534173A (zh) | 2018-01-02 |
EP3286793B1 (de) | 2020-01-15 |
US20180090775A1 (en) | 2018-03-29 |
US20200153009A1 (en) | 2020-05-14 |
WO2016169539A1 (de) | 2016-10-27 |
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