Origin of stabilization and destabilization in solid-state redox reaction of oxide ions for lithium-ion batteries

Naoaki Yabuuchi (), Masanobu Nakayama, Mitsue Takeuchi, Shinichi Komaba, Yu Hashimoto, Takahiro Mukai, Hiromasa Shiiba, Kei Sato, Yuki Kobayashi, Aiko Nakao, Masao Yonemura, Keisuke Yamanaka, Kei Mitsuhara and Toshiaki Ohta
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Naoaki Yabuuchi: Tokyo Denki University
Masanobu Nakayama: Frontier Research Institute for Materials Science, Nagoya Institute of Technology, Gokiso-cho, Showa-ku
Mitsue Takeuchi: Tokyo University of Science
Shinichi Komaba: Tokyo University of Science
Yu Hashimoto: Frontier Research Institute for Materials Science, Nagoya Institute of Technology, Gokiso-cho, Showa-ku
Takahiro Mukai: Frontier Research Institute for Materials Science, Nagoya Institute of Technology, Gokiso-cho, Showa-ku
Hiromasa Shiiba: Frontier Research Institute for Materials Science, Nagoya Institute of Technology, Gokiso-cho, Showa-ku
Kei Sato: Tokyo Denki University
Yuki Kobayashi: Tokyo Denki University
Aiko Nakao: Bio-engineering Lab.
Masao Yonemura: Institute of Materials Structure Science (IMSS), High Energy Accelerator Research Organization (KEK)
Keisuke Yamanaka: SR Center, Ritsumeikan University
Kei Mitsuhara: SR Center, Ritsumeikan University
Toshiaki Ohta: SR Center, Ritsumeikan University

Nature Communications, 2016, vol. 7, issue 1, 1-10

Abstract: Abstract Further increase in energy density of lithium batteries is needed for zero emission vehicles. However, energy density is restricted by unavoidable theoretical limits for positive electrodes used in commercial applications. One possibility towards energy densities exceeding these limits is to utilize anion (oxide ion) redox, instead of classical transition metal redox. Nevertheless, origin of activation of the oxide ion and its stabilization mechanism are not fully understood. Here we demonstrate that the suppression of formation of superoxide-like species on lithium extraction results in reversible redox for oxide ions, which is stabilized by the presence of relatively less covalent character of Mn4+ with oxide ions without the sacrifice of electronic conductivity. On the basis of these findings, we report an electrode material, whose metallic constituents consist only of 3d transition metal elements. The material delivers a reversible capacity of 300 mAh g−1 based on solid-state redox reaction of oxide ions.

Date: 2016
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DOI: 10.1038/ncomms13814

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