JP5048322B2 - セリア系電解質の高密度化 - Google Patents
セリア系電解質の高密度化 Download PDFInfo
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- JP5048322B2 JP5048322B2 JP2006506020A JP2006506020A JP5048322B2 JP 5048322 B2 JP5048322 B2 JP 5048322B2 JP 2006506020 A JP2006506020 A JP 2006506020A JP 2006506020 A JP2006506020 A JP 2006506020A JP 5048322 B2 JP5048322 B2 JP 5048322B2
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- 239000003792 electrolyte Substances 0.000 title claims description 96
- CETPSERCERDGAM-UHFFFAOYSA-N ceric oxide Chemical compound O=[Ce]=O CETPSERCERDGAM-UHFFFAOYSA-N 0.000 title claims description 16
- 229910000422 cerium(IV) oxide Inorganic materials 0.000 title claims description 16
- 238000000280 densification Methods 0.000 title description 10
- 150000001768 cations Chemical class 0.000 claims description 95
- 238000000034 method Methods 0.000 claims description 35
- 238000005245 sintering Methods 0.000 claims description 29
- 239000000758 substrate Substances 0.000 claims description 28
- 229910052751 metal Inorganic materials 0.000 claims description 25
- 239000002184 metal Substances 0.000 claims description 25
- 238000004519 manufacturing process Methods 0.000 claims description 15
- 230000008569 process Effects 0.000 claims description 15
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims description 9
- 239000001301 oxygen Substances 0.000 claims description 9
- 229910052760 oxygen Inorganic materials 0.000 claims description 9
- 239000012535 impurity Substances 0.000 claims description 8
- 239000000463 material Substances 0.000 claims description 2
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 2
- 238000007792 addition Methods 0.000 description 14
- 239000008188 pellet Substances 0.000 description 12
- 230000003647 oxidation Effects 0.000 description 8
- 238000007254 oxidation reaction Methods 0.000 description 8
- 239000012300 argon atmosphere Substances 0.000 description 6
- 230000000694 effects Effects 0.000 description 6
- 238000011109 contamination Methods 0.000 description 5
- 239000011888 foil Substances 0.000 description 5
- 239000000843 powder Substances 0.000 description 5
- 230000002411 adverse Effects 0.000 description 4
- 238000006243 chemical reaction Methods 0.000 description 4
- 239000000446 fuel Substances 0.000 description 4
- 238000012545 processing Methods 0.000 description 4
- 229910001220 stainless steel Inorganic materials 0.000 description 4
- 229910052723 transition metal Inorganic materials 0.000 description 4
- -1 transition metal cations Chemical class 0.000 description 4
- 229910002484 Ce0.9Gd0.1O1.95 Inorganic materials 0.000 description 3
- 229910052804 chromium Inorganic materials 0.000 description 3
- 239000007789 gas Substances 0.000 description 3
- 229910052742 iron Inorganic materials 0.000 description 3
- 230000009467 reduction Effects 0.000 description 3
- 125000002091 cationic group Chemical group 0.000 description 2
- 230000008859 change Effects 0.000 description 2
- 230000001627 detrimental effect Effects 0.000 description 2
- 238000010586 diagram Methods 0.000 description 2
- 238000002474 experimental method Methods 0.000 description 2
- 229910052748 manganese Inorganic materials 0.000 description 2
- 239000012528 membrane Substances 0.000 description 2
- 230000005012 migration Effects 0.000 description 2
- 238000013508 migration Methods 0.000 description 2
- 239000000203 mixture Substances 0.000 description 2
- 239000007787 solid Substances 0.000 description 2
- OVSKIKFHRZPJSS-UHFFFAOYSA-N 2,4-D Chemical compound OC(=O)COC1=CC=C(Cl)C=C1Cl OVSKIKFHRZPJSS-UHFFFAOYSA-N 0.000 description 1
- 229910018072 Al 2 O 3 Inorganic materials 0.000 description 1
- 229910001030 Iron–nickel alloy Inorganic materials 0.000 description 1
- 239000000654 additive Substances 0.000 description 1
- 230000000996 additive effect Effects 0.000 description 1
- 150000001450 anions Chemical class 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- VNNRSPGTAMTISX-UHFFFAOYSA-N chromium nickel Chemical compound [Cr].[Ni] VNNRSPGTAMTISX-UHFFFAOYSA-N 0.000 description 1
- 239000011248 coating agent Substances 0.000 description 1
- 238000000576 coating method Methods 0.000 description 1
- 230000007423 decrease Effects 0.000 description 1
- 238000000151 deposition Methods 0.000 description 1
- 230000006866 deterioration Effects 0.000 description 1
- 238000009826 distribution Methods 0.000 description 1
- 238000000462 isostatic pressing Methods 0.000 description 1
- 238000005259 measurement Methods 0.000 description 1
- 230000007246 mechanism Effects 0.000 description 1
- 229910000000 metal hydroxide Inorganic materials 0.000 description 1
- 150000004692 metal hydroxides Chemical class 0.000 description 1
- 229910044991 metal oxide Inorganic materials 0.000 description 1
- 150000004706 metal oxides Chemical class 0.000 description 1
- 238000003801 milling Methods 0.000 description 1
- 229910001120 nichrome Inorganic materials 0.000 description 1
- RJSRQTFBFAJJIL-UHFFFAOYSA-N niobium titanium Chemical compound [Ti].[Nb] RJSRQTFBFAJJIL-UHFFFAOYSA-N 0.000 description 1
- 238000005457 optimization Methods 0.000 description 1
- 238000013386 optimize process Methods 0.000 description 1
- 239000002245 particle Substances 0.000 description 1
- 230000001737 promoting effect Effects 0.000 description 1
- 230000001681 protective effect Effects 0.000 description 1
- 238000005204 segregation Methods 0.000 description 1
- 239000010935 stainless steel Substances 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 230000002194 synthesizing effect Effects 0.000 description 1
- 230000008719 thickening Effects 0.000 description 1
- 238000003466 welding Methods 0.000 description 1
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Description
製造した電解質中の二価のカチオンの濃度を決定することと;
製造した電解質中の三価のカチオンの濃度を決定することと、前記二価のカチオンの濃度から三価のカチオンの調整された濃度を差し引いて二価のカチオンの有効濃度を出すことと
を含む、製造した電解質中の二価のカチオンの有効濃度の決定方法が提供される。三価のカチオンの悪影響のために、以下に記載するように、測定された濃度に5から10の間のファクターを掛ける必要がある。
電解質に付属した金属基板又は該基板上の酸化物層によって生成した蒸気から二価のカチオンを受け取ること;
基板材料中の三価のカチオンを二価のカチオンに還元すること;又は
製造の前又は間に二価のカチオンを電解質に特別に添加すること;
の1つ以上によって二価のカチオンの濃度を上昇させることを含む。
図1は、カチオンを0、1%及び2%添加したセリア系電解質ペレットの焼結特性を示し;
図2は、カチオンを0及び0.1%添加したセリア系電解質ペレットの焼結特性を示し;
図3は、金属箔で支持された厚膜のセル組立体の略図である。
[ME 2+]=[MA 2+]+[MI 2+]−Y[MI 3+] ・・・ (A)
Claims (13)
- (0.01−[M I 2+ ]+Y[M I 3+ ])≦ [M A 2+ ] ≦(0.1−[M I 2+ ]+Y[M I 3+ ])
(式中、[M A 2+ ]は、焼結プロセスの前に電解質に添加された二価のカチオンのモル%濃度を示し、
[M I 2+ ]は、電解質に二価のカチオンを添加することなく製造する場合に製造される電解質中に存在することが決定された二価のカチオンのモル%濃度を示し、
[M I 3+ ]は、電解質に二価のカチオンを添加することなく製造する場合に製造される電解質中に存在することが決定された三価のカチオンのモル%濃度を示し、
Yは、前記製造される電解質に対して経験的に決定される5から10の間の数である)になるように、焼結プロセスの前に二価のカチオンの電解質への添加を調整する及び/又は焼結プロセスの条件を調整することによって、製造した電解質中の二価及び三価のカチオンの濃度をコントロールし、
該電解質を1200℃以下で焼結する
ことを特徴とする、理論密度の97%より高い密度を有する焼結されたセリア系電解質の焼結プロセスによる製造方法。 - 焼結プロセスの条件をコントロールして、電解質中の三価のカチオン不純物の少なくとも一部を二価のカチオンに還元することを特徴とする請求項1に記載の方法。
- 焼結プロセスの条件をコントロールして適切な酸素又は水圧力を形成し、適切な量の三価のカチオン不純物を二価のカチオンに還元することを特徴とする請求項2に記載の方法。
- 前記電解質を基板上に設け、該基板の材料を選択して、電解質中における二価のカチオンの濃度及び三価のカチオンの濃度が要求される値になるようにすることを特徴とする請求項1,請求項2又は請求項3に記載の方法。
- 前記電解質と前記基板との間に電極を設けることを特徴とする請求項4に記載の方法。
- 前記電解質中の二価のカチオンの少なくとも一部が、金属基板又は金属基板上の酸化物層から生成した蒸気を起源とすることを特徴とする請求項1〜5のいずれか一項に記載の方法。
- 焼結プロセスの前に、前記電解質に二価のカチオンを加えることを特徴とする請求項1〜6のいずれかに記載の方法。
- (0.02−[M I 2+ ]+Y[M I 3+ ])≦ [M A 2+ ] ≦(0.09−[M I 2+ ]+Y[M I 3+ ])
になるように、製造された電解質中における二価及び三価のカチオンの濃度をコントロールすることを特徴とする請求項1〜7のいずれかに記載の方法。 - (0.03−[M I 2+ ]+Y[M I 3+ ])≦ [M A 2+ ] ≦(0.08−[M I 2+ ]+Y[M I 3+ ])
になるように、製造された電解質中における二価及び三価のカチオンの濃度をコントロールすることを特徴とする請求項8に記載の方法。 - 前記電解質を1100℃以下で焼結することを特徴とする請求項1〜9のいずれかに記載の方法。
- 前記電解質を1050℃以下で焼結することを特徴とする請求項10に記載の方法。
- 前記電解質を1000℃以下で焼結することを特徴とする請求項11に記載の方法。
- 前記電解質を厚膜として設けることを特徴とする請求項1〜12のいずれか一項に記載の方法。
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GB0308215A GB2400486B (en) | 2003-04-09 | 2003-04-09 | Densification of ceria based electrolytes |
PCT/GB2004/001293 WO2004089848A1 (en) | 2003-04-09 | 2004-03-25 | Densification of ceria based electrolytes |
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KR100836383B1 (ko) * | 2004-10-15 | 2008-06-09 | 마쯔시다덴기산교 가부시키가이샤 | 연료전지 시스템 |
WO2008003976A1 (en) | 2006-07-07 | 2008-01-10 | Ceres Intellectual Property Company Limited | Metal substrate for fuel cells |
US9120245B1 (en) | 2007-05-09 | 2015-09-01 | The United States Of America As Represented By The Secretary Of The Air Force | Methods for fabrication of parts from bulk low-cost interface-defined nanolaminated materials |
US8617456B1 (en) | 2010-03-22 | 2013-12-31 | The United States Of America As Represented By The Secretary Of The Air Force | Bulk low-cost interface-defined laminated materials and their method of fabrication |
US9162931B1 (en) * | 2007-05-09 | 2015-10-20 | The United States Of America As Represented By The Secretary Of The Air Force | Tailored interfaces between two dissimilar nano-materials and method of manufacture |
KR101478207B1 (ko) * | 2007-11-23 | 2015-01-02 | 삼성전자주식회사 | 이동통신 단말에서 블루투스를 이용하여 자바푸시를요구하는 기기들을 식별하기 위한 방법 및 장치 |
GB2461115A (en) | 2008-04-23 | 2009-12-30 | Ceres Power Ltd | Fuel Cell Module Support |
US9093674B2 (en) | 2008-08-21 | 2015-07-28 | Ceres Intellectual Property Company Limited | Fuel cell stack flow hood air flow using an air distribution device |
FR2948821B1 (fr) | 2009-08-03 | 2011-12-09 | Commissariat Energie Atomique | Cellule electrochimique a metal support et son procede de fabrication |
CN101654366B (zh) * | 2009-09-10 | 2012-10-24 | 中国矿业大学(北京) | 复合助烧剂及其用于低温制备纳米晶陶瓷的方法 |
DE102012211669A1 (de) * | 2012-07-04 | 2014-01-09 | Behr Gmbh & Co. Kg | Klimaanlage |
GB2517927B (en) | 2013-09-04 | 2018-05-16 | Ceres Ip Co Ltd | Process for forming a metal supported solid oxide fuel cell |
GB2517928B (en) | 2013-09-04 | 2018-02-28 | Ceres Ip Co Ltd | Metal supported solid oxide fuel cell |
EP3117477B1 (en) | 2014-03-12 | 2018-12-19 | Ceres Intellectual Property Company Limited | Fuel cell stack arrangement |
GB2534124B (en) | 2014-12-19 | 2017-04-19 | Ceres Ip Co Ltd | A swirl burner assembly and method |
US11527766B2 (en) | 2014-12-19 | 2022-12-13 | Ceres Intellectual Property Company Limited | Fuel cell system and tail gas burner assembly and method |
GB2563848B (en) | 2017-06-26 | 2022-01-12 | Ceres Ip Co Ltd | Fuel cell stack assembly |
GB201913907D0 (en) | 2019-09-26 | 2019-11-13 | Ceres Ip Co Ltd | Fuel cell stack assembly apparatus and method |
GB201915294D0 (en) | 2019-10-22 | 2019-12-04 | Ceres Ip Co Ltd | Alignment apparatus and methods of alignment |
GB201915438D0 (en) | 2019-10-24 | 2019-12-11 | Ceres Ip Co Ltd | Metal-supported cell unit |
GB2591462B (en) | 2020-01-27 | 2022-04-20 | Ceres Ip Co Ltd | Interlayer for solid oxide cell |
GB202009687D0 (en) | 2020-06-25 | 2020-08-12 | Ceres Ip Co Ltd | Layer |
WO2023078940A1 (en) | 2021-11-08 | 2023-05-11 | Rhodia Operations | Cerium-gadolinium composite oxide |
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GB205291A (en) | 1922-09-07 | 1923-10-18 | Francis Mcnally | Improvements in thermometers |
US5403461A (en) * | 1993-03-10 | 1995-04-04 | Massachusetts Institute Of Technology | Solid electrolyte-electrode system for an electrochemical cell |
JPH092873A (ja) * | 1995-01-10 | 1997-01-07 | Tosoh Corp | ホタル石型セリア系固体電解質 |
US5665482A (en) * | 1995-01-10 | 1997-09-09 | Tosoh Corporation | Fluorite structure type ceria type solid electrolyte |
JPH10154523A (ja) * | 1996-09-27 | 1998-06-09 | Tosoh Corp | 欠陥ホタル石型セリア系固体電解質 |
ATE228982T1 (de) * | 1998-11-13 | 2002-12-15 | Eidgenoess Tech Hochschule | Verfahren zur herstellung von dotierter ceroxidkeramik |
CN1150647C (zh) * | 2000-02-16 | 2004-05-19 | 刘向荣 | 中温氧化物燃料电池的复合陶瓷材料 |
ES2344545T3 (es) * | 2000-03-10 | 2010-08-31 | Danmarks Tekniske Universitet | Un metodo de fabricacion de una celula de combustible de oxido solido. |
JP4352594B2 (ja) * | 2000-03-15 | 2009-10-28 | 三菱マテリアル株式会社 | 酸化物イオン伝導体及びその製造方法並びにこれを用いた燃料電池 |
GB2368450B (en) | 2000-10-25 | 2004-05-19 | Imperial College | Fuel cells |
US6770392B2 (en) * | 2001-04-27 | 2004-08-03 | Air Products And Chemicals, Inc. | Ceria based solid electrolytes |
GB2386126B (en) * | 2002-03-06 | 2006-03-08 | Ceres Power Ltd | Forming an impermeable sintered ceramic electrolyte layer on a metallic foil substrate for solid oxide fuel cell |
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KR101065949B1 (ko) | 2011-09-19 |
EA200501588A1 (ru) | 2006-04-28 |
BRPI0409093B1 (pt) | 2013-08-27 |
GB2400486B (en) | 2006-05-10 |
AU2004228427B2 (en) | 2009-09-17 |
US7947212B2 (en) | 2011-05-24 |
WO2004089848A1 (en) | 2004-10-21 |
EP1608605A1 (en) | 2005-12-28 |
JP2006523002A (ja) | 2006-10-05 |
ZA200508144B (en) | 2006-10-25 |
CA2521901C (en) | 2011-09-06 |
EA009103B1 (ru) | 2007-10-26 |
EP1608605B1 (en) | 2013-08-28 |
BRPI0409093A (pt) | 2006-04-11 |
US20110177427A1 (en) | 2011-07-21 |
DK1608605T3 (da) | 2013-12-09 |
GB0308215D0 (en) | 2003-05-14 |
HK1069680A1 (en) | 2005-05-27 |
GB2400486A (en) | 2004-10-13 |
CN1771212A (zh) | 2006-05-10 |
CN100381395C (zh) | 2008-04-16 |
AU2004228427A1 (en) | 2004-10-21 |
KR20060012271A (ko) | 2006-02-07 |
CA2521901A1 (en) | 2004-10-21 |
MXPA05010789A (es) | 2006-03-30 |
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