Joint Cationic and Anionic Redox Chemistry for Advanced Mg Batteries.

Minglei Mao, Yuxin Tong, Qinghua Zhang, Yong-Sheng Hu, Hong Li, Xuejie Huang, Liquan Chen, Lin Gu, Liumin Suo
Author Information
  1. Minglei Mao: Beijing Advanced Innovation Center for Materials Genome Engineering, Key Laboratory for Renewable Energy, Beijing Key Laboratory for New Energy Materials and Devices, Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China. ORCID
  2. Yuxin Tong: Beijing Advanced Innovation Center for Materials Genome Engineering, Key Laboratory for Renewable Energy, Beijing Key Laboratory for New Energy Materials and Devices, Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China.
  3. Qinghua Zhang: Beijing Advanced Innovation Center for Materials Genome Engineering, Key Laboratory for Renewable Energy, Beijing Key Laboratory for New Energy Materials and Devices, Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China.
  4. Yong-Sheng Hu: Beijing Advanced Innovation Center for Materials Genome Engineering, Key Laboratory for Renewable Energy, Beijing Key Laboratory for New Energy Materials and Devices, Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China. ORCID
  5. Hong Li: Beijing Advanced Innovation Center for Materials Genome Engineering, Key Laboratory for Renewable Energy, Beijing Key Laboratory for New Energy Materials and Devices, Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China. ORCID
  6. Xuejie Huang: Beijing Advanced Innovation Center for Materials Genome Engineering, Key Laboratory for Renewable Energy, Beijing Key Laboratory for New Energy Materials and Devices, Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China. ORCID
  7. Liquan Chen: Beijing Advanced Innovation Center for Materials Genome Engineering, Key Laboratory for Renewable Energy, Beijing Key Laboratory for New Energy Materials and Devices, Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China.
  8. Lin Gu: Beijing Advanced Innovation Center for Materials Genome Engineering, Key Laboratory for Renewable Energy, Beijing Key Laboratory for New Energy Materials and Devices, Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China. ORCID
  9. Liumin Suo: Beijing Advanced Innovation Center for Materials Genome Engineering, Key Laboratory for Renewable Energy, Beijing Key Laboratory for New Energy Materials and Devices, Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China. ORCID

Abstract

Lack of appropriate cathodes severely restrains the development of high-energy Mg batteries. In this work, we proposed joint cationic and anionic redox chemistry of transition-metal (TM) sulfides as the most promising way out. A series of solid-solution pyrite FeCoS (0 ≤ ≤ 1) was specially designed, in which S 3p electrons pour into the d bands of Fe and Co, generating redox-active dimerized (S). The FeCoS sample is highlighted to deliver a high specific energy of 240 Wh/kg at room temperature involving both cationic (Fe and Co) and anionic (S) redox. The highly delocalized electronic clouds in pyrite structures comfortably accommodate the charge of Mg, contributing to the fast kinetics and the superior cycling stability of the FeCoS. It is anticipated that the joint cationic and anionic redox chemistry proposed in this work would be the ultimate answer for designing high-energy cathodes for advanced Mg batteries.

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