Hydride in BaTiO<sub>2.5</sub>H<sub>0.5</sub>: A Labile Ligand in Solid State Chemistry
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- Naoya Masuda
- Department of Energy and Hydrocarbon Chemistry, Graduate School of Engineering, Kyoto University, Nishikyo-ku, Kyoto 615-8510, Japan
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- Yoji Kobayashi
- Department of Energy and Hydrocarbon Chemistry, Graduate School of Engineering, Kyoto University, Nishikyo-ku, Kyoto 615-8510, Japan
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- Olivier Hernandez
- Institut des Sciences Chimiques de Rennes, UMR CNRS 6226, Université de Rennes 1, Bâtiment 10B, Campus de Beaulieu, Rennes F-35042, France
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- Thierry Bataille
- Institut des Sciences Chimiques de Rennes, UMR CNRS 6226, Université de Rennes 1, Bâtiment 10B, Campus de Beaulieu, Rennes F-35042, France
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- Serge Paofai
- Institut des Sciences Chimiques de Rennes, UMR CNRS 6226, Université de Rennes 1, Bâtiment 10B, Campus de Beaulieu, Rennes F-35042, France
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- Hajime Suzuki
- Department of Energy and Hydrocarbon Chemistry, Graduate School of Engineering, Kyoto University, Nishikyo-ku, Kyoto 615-8510, Japan
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- Clemens Ritter
- Institut Laue-Langevin, 6, rue Jules Horowitz, Grenoble 38000, France
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- Naoki Ichijo
- Department of Chemistry, Graduate School of Science, Kyoto University, Sakyo-ku, Kyoto 606-8502, Japan
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- Yasuto Noda
- Department of Chemistry, Graduate School of Science, Kyoto University, Sakyo-ku, Kyoto 606-8502, Japan
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- Kiyonori Takegoshi
- Department of Chemistry, Graduate School of Science, Kyoto University, Sakyo-ku, Kyoto 606-8502, Japan
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- Cédric Tassel
- Department of Energy and Hydrocarbon Chemistry, Graduate School of Engineering, Kyoto University, Nishikyo-ku, Kyoto 615-8510, Japan
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- Takafumi Yamamoto
- Department of Energy and Hydrocarbon Chemistry, Graduate School of Engineering, Kyoto University, Nishikyo-ku, Kyoto 615-8510, Japan
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- Hiroshi Kageyama
- Department of Energy and Hydrocarbon Chemistry, Graduate School of Engineering, Kyoto University, Nishikyo-ku, Kyoto 615-8510, Japan
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説明
In synthesizing mixed anion oxides, direct syntheses have often been employed, usually involving high temperature and occasionally high pressure. Compared with these methods, here we show how the use of a titanium perovskite oxyhydride (BaTiO2.5H0.5) as a starting material enables new multistep low temperature topochemical routes to access mixed anion compounds. Similar to labile ligands in inorganic complexes, the lability of H(-) provides the necessary reactivity for syntheses, leading to reactions and products previously difficult to obtain. For example, BaTiO2.5N0.2 can be prepared with the otherwise inert N2 gas at 400-600 °C, in marked contrast with currently available oxynitride synthetic routes. F(-)/H(-) exchange can also be accomplished at 150 °C, yielding the oxyhydride-fluoride BaTi(O, H, F)3. For BaTiO2.4D0.3F0.3, we find evidence that further anionic exchange with OD(-) yields BaTiO2.4(D(-))0.26(OD(-))0.34, which implies stable coexistence of H(+) and H(-) at ambient conditions. Such an arrangement is thermodynamically unstable and would be difficult to realize otherwise. These results show that the labile nature of hydride imparts reactivity to oxide hosts, enabling it to participate in new multistep reactions and form new materials.
収録刊行物
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- Journal of the American Chemical Society
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Journal of the American Chemical Society 137 (48), 15315-15321, 2015-11-30
American Chemical Society (ACS)
