Development of fast oxide ion conductor and application for new electrochemical devices

快速氧化物离子导体的研制及其在新型电化学器件中的应用

• 批准号: 11102006
• 负责人: TAKITA Yusaku
• 金额: $ 209.79万
• 依托单位: Oita University
• 依托单位国家: 日本
• 项目类别: Grant-in-Aid for Specially Promoted Research
• 财政年份: 1999
• 资助国家: 日本
• 起止时间: 1999 至 2003
• 项目状态: 已结题
• 来源: https://kaken.nii.ac.jp/grant/KAKENHI-PROJECT-11102006/
• 关键词: Oxide ion conductor; Nanometer size effects; Solid Oxide Fuel Cells; Air Separation; Electrode catalyst; Diffusion Coeficient; 酸素イオン伝導; LaGaO_3; 酸化物電解質燃料電池; 超薄膜; La_2GeO_5; 酸素イオン伝導体; LaF_3; 酸素透過膜; 炭化水素センサー; 排ガスモニター; ペロブスカイト; 同位体拡散; 部分酸化

In this study, new fast oxide ion conducting oxide was investigated and it was found that mixed oxide of La_2GeO_5, LaOF, and Fe heavily doped LaGaO_3 based oxide exhibits extremely fast oxide ion conductivity comparing with the conventional materials. Furthermore, conduction mechanisms in LaGaO_3 based oxide was studied in details and it was found that oxide ion conductivity in LaGaO_3 based oxide was improved by doping Fe, Co, and Ni. Partial electronic conduction was also observed. However, if the amount of doped Co, Ni, or Fe is small, the contribution of electronic charge carrier is not significant. In particular, it was found that the oxide ion conductivity in LaGaO_3 based oxide greatly improved by doping Fe. In agreement with the improved oxide ion conductivity, power density of the solid oxide fuel cells is also improved by using Fe, Co, or Ni doped LaGaO_3 for electrolyte. On the other hand, crystal structural analysis of La_2GeO_5 based oxide suggests the large anisotropic oxide ion conductivity is occurred in this oxide. The high oxide ion conductivity in this La_2GeO_5 system seems to result from the high mobility of oxide ion. Making thin film of La_2GeO_5 based oxide with nanometer level thickness was successfully prepared by Laser Abrasion Methods. It was found that the unusual increase in oxide ion conductivity is achieved as the thickness of the La_2GeO_5 based oxide film decreased to a nanometer size. Furthermore, accumulation of La_2GeO_5 nanometer sized film on LaGaO_3 based oxide film with nanometer size thickness is effective for increasing the oxide ion conductivity.

本论文研究了新型快速氧化物离子导电材料，发现La_2GeO_5、LaOF和Fe重掺杂LaGaO_3基氧化物的混合氧化物具有比传统材料更快的氧化物离子导电性。此外，还对LaGaO_3基氧化物的导电机理进行了详细的研究，发现掺杂Fe、Co、Ni等元素可以提高LaGaO_3基氧化物的氧离子电导率。还观察到部分电子传导。然而，如果掺杂的Co、Ni或Fe的量小，则电子电荷载流子的贡献不显著。特别地，发现掺杂Fe大大提高了LaGaO_3基氧化物的氧离子电导率。在提高氧离子电导率的同时，掺杂Fe、Co或Ni的LaGaO_3电解质也提高了固体氧化物燃料电池的功率密度。另一方面，La_2GeO_5基氧化物的晶体结构分析表明，该氧化物具有较大的各向异性氧离子电导率。La_2GeO_5体系中高的氧离子电导率可能是由于氧离子的高迁移率所致。用激光研磨法成功地制备了纳米级La_2GeO_5基氧化物薄膜。结果表明，当La_2GeO_5基氧化膜厚度减小到纳米级时，氧化物离子电导率显著增加。在LaGaO_3基纳米氧化膜上沉积La_2GeO_5纳米膜对提高氧离子电导率是有效的。

项目成果

T.Ishihara, Y.Tsuruta, H.Nishiguchi, Y.Takita: "Fe doped LaGaO_3 based perovskite oxide as an oxygen separating membrane for CH_4 partial oxidation"Ceramic Transactions,. 127. 69-77 (2002)

T.Ishihara，Y.Tsuruta，H.Nishiguchi，Y.Takita：“Fe掺杂LaGaO_3基钙钛矿氧化物作为CH_4部分氧化的氧分离膜”，《陶瓷汇刊》，。

S.Wang, T.Ishihara, Y.Takita: "Dimethyl Ether Fueled Intermediate Temperature Solid Oxide Fuel Cell Using LaGaO_3 Based Perovskite Electrolytes"Electrochem. & Solid-State Lett.,. 5. A177-A180 (2002)

S.Wang、T.Ishihara、Y.Takita：“使用 LaGaO_3 基钙钛矿电解质的二甲醚燃料中温固体氧化物燃料电池”Electrochem。

T.Ishihara, S.Fukui, H.Nishiguchi, Y.Takita: "Mixed electronic-oxide ionic conductor of BaCO_3 doped with La for cathode of intermediate Temperature operating solid oxide fuel cell"Solid Sate Ionics. 152-154. 609-615 (2002)

T.Ishihara、S.Fukui、H.Nishiguchi、Y.Takita：“BaCO_3 混合电子氧化物离子导体，掺杂 La，用于中温固体氧化物燃料电池的阴极”Solid Sate Ionics。

T.Ishihara, T.Shibayama, H.Nishiguchi, Y.Takita: "Oxide Ion Conductivity in La_<0.8>Sr_<0.2>Ga_<0.8>Mg_<0.2-X>Ni_XO_3 Perovskite Oxide and Application for the Electrolyte of Solid Oxide Fuel Cells"J. Materials Science. 36. 1051-1182 (2001)

T.Ishihara，T.Shibayama，H.Nishiguchi，Y.Takita：“La_<0.8>Sr_<0.2>Ga_<0.8>Mg_<0.2-X>Ni_XO_3钙钛矿氧化物中的氧化物离子电导率及其在固体氧化物电解质中的应用

石原達己: "季刊化学総説No.48「新型電池の材料化学」"日本化学会(印刷中).

Tatsumi Ishihara：“化学评论季刊第 48 期‘新型电池的材料化学’”，日本化学会（出版中）。