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Protonic conduction, crystal and electronic structures of La$$_{0.9}$$Ba$$_{1.1}$$Ga$$_{0.95}$$Mg$$_{0.05}$$O$$_{4-delta}$$

La$$_{0.9}$$Ba$$_{1.1}$$Ga$$_{0.95}$$Mg$$_{0.05}$$O$$_{4-delta}$$のプロトン伝導、結晶/電子構造の解析

浜尾 尚樹*; 北村 尚斗*; 伊藤 孝憲*; 井川 直樹   ; 井手本 康*; 大道 博行; 加来 正典*; 窪寺 昌一*

Hamao, Naoki*; Kitamura, Naoto*; Ito, Takanori*; Igawa, Naoki; Idemoto, Yasushi*; Daido, Hiroyuki; Kaku, Masanori*; Kubodera, Masakazu*

燃料電池用固体電解質材料、La$$_{0.9}$$Ba$$_{1.1}$$Ga$$_{0.95}$$Mg$$_{0.05}$$O$$_{4-delta}$$を固相反応法で合成し、電気伝導度やRietveld/最大エントロピー法による結晶構造解析を行った。基本材料であるLaBaGaO$$_{4}$$の一部をBaやMgで置換することで、プロトン伝導度が向上した。Rietveld/最大エントロピー法解析の結果、1000Kまでの温度ではLa$$_{0.9}$$Ba$$_{1.1}$$Ga$$_{0.95}$$Mg$$_{0.05}$$O$$_{4-delta}$$はLaBaGaO$$_{4}$$と同じ結晶構造を有すること、プロトンはO3サイト近傍に配置し、この酸素と水素結合していることがわかった。

La$$_{0.9}$$Ba$$_{1.1}$$Ga$$_{0.95}$$Mg$$_{0.05}$$O$$_{4-delta}$$ which is one of the candidates for solid electrolyte of solid oxide fuel cell was synthesized by means of a conventional solid-state reaction, and investigated by conductivity measurements, the Rietveld and maximum entropy method analyses using neutron and synchrotron X-ray diffraction data. Conductivity measurements indicated that simultaneous Ba and Mg substitutions for LaBaGaO$$_{4}$$ were effective way to improve the protonic conductivity. From the Rietveld and maximum entropy method analyses, it was confirmed that La$$_{0.9}$$Ba$$_{1.1}$$Ga$$_{0.95}$$Mg$$_{0.05}$$O$$_{4-delta}$$ kept the same crystal structure as LaBaGaO$$_{4}$$ even at elevated temperature, i.e. 1000 K, and that protons existed around the O3 site and formed hydrogen bonds. It is also found that oxygens in LaBaGaO$$_{4}$$-based samples formed Ga-O$$_{4}$$ tetrahedra, and the bonding strength was varied by the partial substitutions.

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パーセンタイル:15.53

分野:Chemistry, Physical

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