JP2007515745A - 固体酸化物燃料電池 - Google Patents
固体酸化物燃料電池 Download PDFInfo
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Abstract
【選択図】図1
Description
固体酸化物燃料電池(SOFC)は高効率及び低汚染物質放出で化学的エネルギーを電気的エネルギーに変換する。“生エネルギー(green energy)”の導入は魅力的なシナリオであるかのように見えるかもしれないがその実施は技術的及び経済的な困難が付きまとう。
更に、ニッケルサーメットはレドックス耐性が乏しいために多くの中及び小規模の応用が妨げられている。このように、S.Tao及びJ.T.S Irvineの、Natural Materials、2、320-323、2003により報告されているように代替のアノード系を見出すことにかなりの関心がある。
好ましくは、本発明のアノードはコバルト及び鉄を含むセラミックを含有する。
M2-xSrxFe2-yCoyO5±δ
(式中、MはCaまたは希土類元素であり;x及びyは独立して0乃至2の間で0及び2を含んでなる値に等しく;そしてδは化学量論からの値である);または
MxSr1-xFe1.5-yCoyO3+δ
(式中、MはCaまたは希土類元素であり;x及びyは独立して0乃至0.7の間で0及び0.7を含んでなる値に等しく;そしてδは化学量論からの値である)を有することができる。
また、本発明によるセラミックは、例えば一般式:La1-xSrxCo1-yFeyO3-δ(式中、x及びyは独立して0乃至1の間で0及び1を含んでなる値に等しく;そしてδは化学量論からの値である)を有するランタン ストロンチウム コバルト 鉄酸化物であり得る。
好ましくは、本発明のアノードは金属を含まない。金属を含まないとは、アノードに存在する元素はいずれも金属形態でないことを意図する。
本発明において有用なドープしたセリアの例は、ガドリニアでドープしたセリア及びサマリアでドープしたセリアである。また、セリアはランタン、イッテルビウム、イットリウム、カルシウム、テルビウム、ネオジム及びジスプロシウムから選択された陽イオンでドープすることができる。
好ましくは、本発明のドープしたセリアはサブミクロンの粒子サイズを有する。より具体的には前記粒子サイズは100nm未満である。
該電解質が支持しない、すなわち電極で支持された、固体酸化物燃料電池の固体酸化物燃料電池配置において、該電解質膜は任意の好ましいセラミック材料、例えば上で述べたドーブしたセリアまたはイットリアで安定化したジルコニア(YSZ)を含有することができる。
少なくとも1種の燃料をコバルト及び鉄の少なくとも1種を含むセラミックを含有し、前記セラミックがドープしたセリアと混合されているアノード、カソード及び前記アノード及び前記カソードの間に配置された少なくとも1種の電解質膜を含有する固体酸化物燃料電池のアノード側へ供給し;
酸化剤を前記固体酸化物燃料電池のカソード側へ供給し;そして
前記少なくとも1種の燃料を前記固体酸化物燃料電池中で酸化してエネルギーを産出する
工程を含有するエネルギーの産出方法に関する。
本発明の方法は適切量の水が水素以外の燃料と組合わせて用いられた場合、アノード側で内部改質相を提供することができる。
図1は模式的にアノード1、カソード2及び電解質膜3を含有する固体酸化物燃料電池を示す。矢印は操作中のアノードからカソードへの電子の流れを示す。
LSCF-CGO-LSCF/CGO
次の構造及び組成を有する固体酸化物電池を作製して試験した。
カソード:組成:LSCF-80
厚さ:〜20μm
電解質膜:組成:CGO-20
厚さ:300μm
アノード:組成:30重量%のCGO-20 + 70重量%のLSCF-80
厚さ:〜20μm
1. 電解質の調製
(a) CGO-20粉末合成
250mlの水中の12.6gのシュウ酸 (Aldrich、99.999%)溶液を水酸化ナトリウム(0.1M)(Aldrich)でpHを6.5とした。8.0gのCe(NO3)3・6H2O(Aldrich、99.99%)及び2.078gのGd(NO3)3・6H2O(Aldrich、99.99%)を50mlの水に添加し、完全に溶解するまで攪拌した。この陽イオン溶液を該シュウ酸溶液へ滴下して、比が1モルCe3+:〜6モルのH2C2O4及び1モルGd3+:〜6モルのH2C2O4を与えた。生成した沈殿物をろ過し、水で3回洗浄し、そして100℃で4時間乾燥した。洗浄に用いた水のpHは6.5までであった。乾燥した粉末を粉砕し、700℃で4時間結晶化した。CGO-20ナノ粉末(4g)が得られた。このナノ粉末は、Scherrerの式:
t = K×λ/(βcosθ)
[式中、Kは平均クリスタリットの形状係数;λは波長;β(rad)は個々の
ピークの半値全幅;そしてθ(rad)はピーク位置(2θ/2)である]
を使用する線の拡がりの測定によるX線回折図(図2)から測定された26nmの粒子サイズを有する。
(b) CGO-20電解質膜の作製
(a)のCGO-20粉末を1,050℃で1時間熱的に処理し、次いで300MPaで一軸的にプレスし、そして得られたペレットを1,450℃で6時間熱的に処理して95%を超える相対密度(実験上の密度/理論上の密度)を有する約300μmの厚さの膜を与えた。
LSFC-80粉末(10g;単ペロブスカイト相、一次粒子平均サイズ9nm、BET表面積:4.12m2/g、Praxair)をボールミルで10mlのエタノール中14時間均一化した。次いで、1gのスラリーをとり、15mlのエタノールを添加してそのスラリーを希釈し、超音波浴中で4時間よく分散させた。得られた溶液を400℃に保たれた該電解質膜上にエアログラフ装置で3分間噴霧した。次いで該カソード及び電極/電解質膜界面を1,100℃で2時間5℃/分の加熱及び冷却ランプ(ramp)の空気条件下で焼結した。
LSFC-80粉末(10g;単ペロブスカイト相、一次粒子平均サイズ9nm、BET表面積:4.12m2/g、Praxair)をめのう乳鉢中でCGO-20[1. (a)-(b)で調製した3g]と均一化した。次いで、該混合物を10mlのエタノール中で14時間ボールミルで摩砕した。 次に1gのスラリーをとり、15mlのエタノールを添加してそのスラリーを希釈し、超音波浴中で4時間よく分散させた。得られた溶液を400℃に保たれた該電解質膜上にエアログラフ装置で3分間噴霧した。次いで該電極及び電極/電解質膜界面を800℃で1時間、そしてそれから1,100℃で2時間5℃/分の加熱及び冷却ランプの空気条件下で焼結した。
電池評価は実質的に乾燥したメタンで以って800℃の温度で操作して行った。その結果を図3に示す。図3において黒及び白抜きの四角はそれぞれ分極曲線及び出力密度曲線を示す。0.6Vで0.3A/cm2に近い電流密度を示した。到達した最大出力密度は170mW/cm2であった。
Claims (30)
- カソード、アノード及び前記カソード及び前記アノードの間に配置された少なくとも一つの電解質膜を含む固体酸化物燃料電池であって、前記アノードがコバルト及び鉄の少なくとも一つを含むセラミックを含有し、前記セラミックがドープしたセリアと混合されている固体酸化物燃料電池。
- 該セラミックがペロブスカイト型構造またはペロブスカイト型関連構造である、請求項1の固体酸化物燃料電池。
- 該セラミックがコバルト及び鉄を含む、請求項1の固体酸化物燃料電池。
- 該セラミックが式:
M2-xSrxFe2-yCoyO5±δ
(式中、MはCaまたは希土類元素であり;x及びyは独立して0乃至2の間で両端を含んでなる値に等しく;そしてδは化学量論からの値である)を有する、請求項1の固体酸化物燃料電池。 - 該セラミックが式:
MxSr1-xFe1.5-yCoyO3+δ
(式中、MはCaまたは希土類元素であり;x及びyは独立して0乃至0.7の間で両端を含んでなる値に等しく;そしてδは化学量論からの値である)を有する、請求項1の固体酸化物燃料電池。 - 該セラミックがLa0.8Sr0.2FeO3である、請求項5の固体酸化物燃料電池。
- 該セラミックがランタン ストロンチウム コバルト 鉄酸化物である、請求項1の固体酸化物燃料電池。
- 該ランタン ストロンチウム コバルト 鉄酸化物が一般式:
La1-xSrxCo1-yFeyO3-δ
(式中、x及びyは独立して0乃至1の間で両端を含んでなる値に等しく;そしてδは化学量論からの値である)を有する、請求項7の固体酸化物燃料電池。 - 該ランタン ストロンチウム コバルト 鉄酸化物が式:
La0.6Sr0.4Co0.2Fe0.8O3-δ
を有する、請求項8の固体酸化物燃料電池。 - 該アノードが金属を含まない、請求項1の固体酸化物燃料電池。
- 該セラミックと該ドープしたセリアとがセラミック対ドープしたセリアの比率が50:50乃至95:5の範囲で混合される、請求項1の固体酸化物燃料電池。
- 該比率が60:40乃至80:20範囲にある、請求項11の固体酸化物燃料電池。
- 該ドープしたセリアがガドリニアでドープしたセリア及びサマリアでドープしたセリアから選択される、請求項1の固体酸化物燃料電池。
- セリアがランタン、イッテルビウム、イットリウム、カルシウム、テルビウム、ネオジム及びジスプロシウムから選択される陽イオンでドープされた、請求項1の固体酸化物燃料電池。
- 該ドープしたセリアが約20モル%の量でドープされた、請求項1の固体酸化物燃料電池。
- 該ドープしたセリアがCe0.8Gd0.2O1.90である、請求項1の固体酸化物燃料電池。
- 該ドープしたセリアがサブミクロンの粒子サイズを有する、請求項1の固体酸化物燃料電池。
- 該ドープしたセリアが100nm未満の粒子サイズを有する、請求項17の固体酸化物燃料電池。
- 該カソードが、
La1-xSrxMnO3-δ
(式中、x及びyは独立して0乃至1の間で両端を含んでなる値に等しく;そしてδは化学量論からの値である)及び
La1-xSrxCo1-yFeyO3-δ
(式中、x及びyは独立して0乃至1の間で両端を含んでなる値に等しく;そしてδは化学量論からの値である)からなる群より選択されたセラミックを含有する、
請求項1の固体酸化物燃料電池。 - 該カソードがドープしたセリアを含有する、請求項1の固体酸化物燃料電池。
- 該電解質膜がドープしたセリアを含有する、請求項1の固体酸化物燃料電池。
- 該電解質膜が支持しない、請求項1の固体酸化物燃料電池。
- 少なくとも1種の燃料をコバルト及び鉄の少なくとも一つを含むセラミックを含有し、前記セラミックがドープしたセリアと混合されているアノード、カソード及び前記アノード及び前記カソードの間に配置された少なくとも一つの電解質膜を含有する固体酸化物燃料電池のアノード側へ供給し;
酸化剤を前記固体酸化物燃料電池のカソード側へ供給し;そして
前記少なくとも1種の燃料を前記固体酸化物燃料電池中で酸化してエネルギーを産出する、
工程を含有するエネルギーの産出方法。 - 該少なくとも1種の燃料が水素である、請求項23の方法。
- 該少なくとも1種の燃料がアルコールである、請求項23の方法。
- 該少なくとも1種の燃料が気体状炭化水素である、請求項23の方法。
- 該炭化水素が実質的に乾燥している、請求項26の方法。
- 該少なくとも1種の燃料が液体状炭化水素である、請求項23の方法。
- 該少なくとも1種の燃料が実質的に乾燥メタンである、請求項23の方法。
- 該燃料が該アノード側で内的に改質される、請求項23の方法。
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KR102159510B1 (ko) | 2019-03-20 | 2020-09-25 | 울산과학기술원 | 용리 및 치환된 전이원소를 가지는 촉매체를 포함하는 전극 소재의 제조 방법 및 이를 이용하여 제조한 전극 소재를 포함하는 금속공기전지, 고체 산화물 연료전지 및 고체 산화물 수전해 셀 |
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KR20130134799A (ko) * | 2012-05-31 | 2013-12-10 | 서울대학교산학협력단 | 메조 기공 구조의 복합분말 제조 방법 및 이를 이용한 고체산화물 연료전지 제조 방법 |
KR102025440B1 (ko) | 2012-05-31 | 2019-09-25 | 서울대학교산학협력단 | 메조 기공 구조의 복합분말 제조 방법 및 이를 이용한 고체산화물 연료전지 제조 방법 |
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JP2020107406A (ja) * | 2018-12-26 | 2020-07-09 | 東邦瓦斯株式会社 | 燃料電池および燃料電池の運転方法 |
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