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Title: Gas phase contributions to topochemical hydride reduction reactions

Abstract

Alkali and alkali earth hydrides have been used as solid state reductants recently to yield many interesting new oxygen-deficient transition metal oxides. These reactions have tacitly been assumed to be a solid phase reaction between the reductant and parent oxide. We have conducted a number of experiments with physical separation between the reductant and oxides, and find that in some cases reduction proceeds even when the reagents are physically separated, implying reactions with in-situ generated H{sub 2} and, to a lesser extent, getter mechanisms. Our findings change our understanding of these topochemical reactions, and should enhance the synthesis of additional new oxides and nanostructures. - Graphical abstract: Topochemical reductions with hydrides: Solid state or gas phase reaction? Display Omitted - Highlights: • SrFeO{sub 2} and LaNiO{sub 2} were prepared by topochemical reduction of oxides. • Separating the reducing agent (CaH{sub 2}, Mg metal) from the oxide still results in reduction. • Such topochemical reactions can occur in the gas phase.

Authors:
 [1];  [2];  [3];  [1];  [1];  [4];  [1];  [1];  [4];
  1. Department of Energy and Hydrocarbon Chemistry, Graduate School of Engineering, Kyoto University, Nishikyo-ku, Kyoto 615-8510 (Japan)
  2. Institute for Integrated Cell-Material Sciences, Kyoto University, Sakyo-ku, Kyoto 606-8502 (Japan)
  3. Institute for Chemical Research, Kyoto University, Gokasho, Uji, Kyoto 611-0011 (Japan)
  4. CREST, Japan Science and Technology Agency (JST), Kawaguchi, Saitama 332-0012 (Japan)
Publication Date:
OSTI Identifier:
22274164
Resource Type:
Journal Article
Journal Name:
Journal of Solid State Chemistry
Additional Journal Information:
Journal Volume: 207; Other Information: Copyright (c) 2013 Elsevier Science B.V., Amsterdam, The Netherlands, All rights reserved.; Country of input: International Atomic Energy Agency (IAEA); Journal ID: ISSN 0022-4596
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; CALCIUM HYDRIDES; NANOSTRUCTURES; OXIDES; OXYGEN; REAGENTS; REDUCING AGENTS; SOLIDS; SYNTHESIS; TRANSITION ELEMENTS

Citation Formats

Kobayashi, Yoji, CREST, Japan Science and Technology Agency, Li, Zhaofei, Hirai, Kei, Tassel, Cédric, The Hakubi Center for Advanced Research, Kyoto University, Yoshida-Ushinomiya-cho, Sakyo-ku, Kyoto 606-8302, Loyer, François, Institut des Sciences Chimiques de Rennes, UMR 6226 Université de Rennes 1-CNRS, équipe CSM, Bât. 10B, Campus de Beaulieu, 263, Avenue du Général Leclerc, 35042 Rennes Cedex, Ichikawa, Noriya, Institute for Chemical Research, Kyoto University, Gokasho, Uji, Kyoto 611-0011, Abe, Naoyuki, Department of Chemistry, Graduate School of Science, Kyoto University, Sakyo-ku, Kyoto 606-8502, Yamamoto, Takafumi, Shimakawa, Yuichi, Institute for Chemical Research, Kyoto University, Gokasho, Uji, Kyoto 611-0011, and others, and. Gas phase contributions to topochemical hydride reduction reactions. United States: N. p., 2013. Web. doi:10.1016/J.JSSC.2013.09.006.
Kobayashi, Yoji, CREST, Japan Science and Technology Agency, Li, Zhaofei, Hirai, Kei, Tassel, Cédric, The Hakubi Center for Advanced Research, Kyoto University, Yoshida-Ushinomiya-cho, Sakyo-ku, Kyoto 606-8302, Loyer, François, Institut des Sciences Chimiques de Rennes, UMR 6226 Université de Rennes 1-CNRS, équipe CSM, Bât. 10B, Campus de Beaulieu, 263, Avenue du Général Leclerc, 35042 Rennes Cedex, Ichikawa, Noriya, Institute for Chemical Research, Kyoto University, Gokasho, Uji, Kyoto 611-0011, Abe, Naoyuki, Department of Chemistry, Graduate School of Science, Kyoto University, Sakyo-ku, Kyoto 606-8502, Yamamoto, Takafumi, Shimakawa, Yuichi, Institute for Chemical Research, Kyoto University, Gokasho, Uji, Kyoto 611-0011, & others, and. Gas phase contributions to topochemical hydride reduction reactions. United States. https://doi.org/10.1016/J.JSSC.2013.09.006
Kobayashi, Yoji, CREST, Japan Science and Technology Agency, Li, Zhaofei, Hirai, Kei, Tassel, Cédric, The Hakubi Center for Advanced Research, Kyoto University, Yoshida-Ushinomiya-cho, Sakyo-ku, Kyoto 606-8302, Loyer, François, Institut des Sciences Chimiques de Rennes, UMR 6226 Université de Rennes 1-CNRS, équipe CSM, Bât. 10B, Campus de Beaulieu, 263, Avenue du Général Leclerc, 35042 Rennes Cedex, Ichikawa, Noriya, Institute for Chemical Research, Kyoto University, Gokasho, Uji, Kyoto 611-0011, Abe, Naoyuki, Department of Chemistry, Graduate School of Science, Kyoto University, Sakyo-ku, Kyoto 606-8502, Yamamoto, Takafumi, Shimakawa, Yuichi, Institute for Chemical Research, Kyoto University, Gokasho, Uji, Kyoto 611-0011, and others, and. 2013. "Gas phase contributions to topochemical hydride reduction reactions". United States. https://doi.org/10.1016/J.JSSC.2013.09.006.
@article{osti_22274164,
title = {Gas phase contributions to topochemical hydride reduction reactions},
author = {Kobayashi, Yoji and CREST, Japan Science and Technology Agency and Li, Zhaofei and Hirai, Kei and Tassel, Cédric and The Hakubi Center for Advanced Research, Kyoto University, Yoshida-Ushinomiya-cho, Sakyo-ku, Kyoto 606-8302 and Loyer, François and Institut des Sciences Chimiques de Rennes, UMR 6226 Université de Rennes 1-CNRS, équipe CSM, Bât. 10B, Campus de Beaulieu, 263, Avenue du Général Leclerc, 35042 Rennes Cedex and Ichikawa, Noriya and Institute for Chemical Research, Kyoto University, Gokasho, Uji, Kyoto 611-0011 and Abe, Naoyuki and Department of Chemistry, Graduate School of Science, Kyoto University, Sakyo-ku, Kyoto 606-8502 and Yamamoto, Takafumi and Shimakawa, Yuichi and Institute for Chemical Research, Kyoto University, Gokasho, Uji, Kyoto 611-0011 and others, and},
abstractNote = {Alkali and alkali earth hydrides have been used as solid state reductants recently to yield many interesting new oxygen-deficient transition metal oxides. These reactions have tacitly been assumed to be a solid phase reaction between the reductant and parent oxide. We have conducted a number of experiments with physical separation between the reductant and oxides, and find that in some cases reduction proceeds even when the reagents are physically separated, implying reactions with in-situ generated H{sub 2} and, to a lesser extent, getter mechanisms. Our findings change our understanding of these topochemical reactions, and should enhance the synthesis of additional new oxides and nanostructures. - Graphical abstract: Topochemical reductions with hydrides: Solid state or gas phase reaction? Display Omitted - Highlights: • SrFeO{sub 2} and LaNiO{sub 2} were prepared by topochemical reduction of oxides. • Separating the reducing agent (CaH{sub 2}, Mg metal) from the oxide still results in reduction. • Such topochemical reactions can occur in the gas phase.},
doi = {10.1016/J.JSSC.2013.09.006},
url = {https://www.osti.gov/biblio/22274164}, journal = {Journal of Solid State Chemistry},
issn = {0022-4596},
number = ,
volume = 207,
place = {United States},
year = {Fri Nov 15 00:00:00 EST 2013},
month = {Fri Nov 15 00:00:00 EST 2013}
}