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タイトル: | Unexpectedly Large Contribution of Oxygen to Charge Compensation Triggered by Structural Disordering: Detailed Experimental and Theoretical Study on a Li₃NbO₄–NiO Binary System |
著者: | Fukuma, Ryutaro Harada, Maho Zhao, Wenwen Sawamura, Miho Noda, Yusuke Nakayama, Masanobu Goto, Masato https://orcid.org/0000-0002-8198-7622 (unconfirmed) Kan, Daisuke Shimakawa, Yuichi https://orcid.org/0000-0003-1019-2512 (unconfirmed) Yonemura, Masao Ikeda, Naohiro Watanuki, Ryuta Andersen, Henrik L. D’Angelo, Anita M. Sharma, Neeraj Park, Jiwon Byon, Hye Ryung Fukuyama, Sayuri Han, Zhenji Fukumitsu, Hitoshi Schulz-Dobrick, Martin Yamanaka, Keisuke Yamagishi, Hirona Ohta, Toshiaki Yabuuchi, Naoaki |
著者名の別形: | 福間, 隆太朗 原田, 真帆 趙, 文文 澤村, 美穂 野田, 祐輔 中山, 将伸 後藤, 真人 菅, 大介 島川, 祐一 米村, 雅雄 池田, 直宏 綿貫, 竜太 福山, 小百合 韓, 貞姫 福満, 仁志 山中, 恵介 山岸, 弘奈 太田, 俊明 藪内, 直明 |
キーワード: | Chemical structure Ions Oxygen Redox reactions Transition metals |
発行日: | 22-Jun-2022 |
出版者: | American Chemical Society (ACS) |
誌名: | ACS Central Science |
巻: | 8 |
号: | 6 |
開始ページ: | 775 |
終了ページ: | 794 |
抄録: | Dependence on lithium-ion batteries for automobile applications is rapidly increasing. The emerging use of anionic redox can boost the energy density of batteries, but the fundamental origin of anionic redox is still under debate. Moreover, to realize anionic redox, many reported electrode materials rely on manganese ions through π-type interactions with oxygen. Here, through a systematic experimental and theoretical study on a binary system of Li₃NbO₄–NiO, we demonstrate for the first time the unexpectedly large contribution of oxygen to charge compensation for electrochemical oxidation in Ni-based materials. In general, for Ni-based materials, e.g., LiNiO₂, charge compensation is achieved mainly by Ni oxidation, with a lower contribution from oxygen. In contrast, for Li₃NbO₄–NiO, oxygen-based charge compensation is triggered by structural disordering and σ-type interactions with nickel ions, which are associated with a unique environment for oxygen, i.e., a linear Ni–O–Ni configuration in the disordered system. Reversible anionic redox with a small hysteretic behavior was achieved for LiNi₂/₃Nb₁/₃O₂ with a cation-disordered Li/Ni arrangement. Further Li enrichment in the structure destabilizes anionic redox and leads to irreversible oxygen loss due to the disappearance of the linear Ni–O–Ni configuration and the formation of unstable Ni ions with high oxidation states. On the basis of these results, we discuss the possibility of using σ-type interactions for anionic redox to design advanced electrode materials for high-energy lithium-ion batteries. |
記述: | 酸素が反応に寄与するニッケル系電池材料 高エネルギー密度リチウム電池実現に期待 --新規不規則岩塩型ニッケル系材料開発と次世代蓄電池への応用--. 京都大学プレスリリース. 2022-05-24. |
著作権等: | © 2022 The Authors. Published by American Chemical Society This article is licensed under the Creative Commons Attribution 4.0 International License. |
URI: | http://hdl.handle.net/2433/274532 |
DOI(出版社版): | 10.1021/acscentsci.2c00238 |
PubMed ID: | 35756387 |
関連リンク: | https://www.kyoto-u.ac.jp/ja/research-news/2022-05-24-0 |
出現コレクション: | 学術雑誌掲載論文等 |
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