Citation: Dixing Ni, Jiarui Qi, Zhi Deng, Dong Ding, Rui Wang, Wenjie Zhou, Sisi Zhou, Yang Sun, Shuai Li, Zhaoxiang Wang. Voltage design and transport channel optimization of anti-perovskite cathode materials: A density functional theory study[J]. Chinese Chemical Letters, ;2025, 36(12): 110683. doi: 10.1016/j.cclet.2024.110683 shu

Voltage design and transport channel optimization of anti-perovskite cathode materials: A density functional theory study

Dixing Ni ^a ,
Jiarui Qi ^a ,
Zhi Deng ^a ,
Dong Ding ^{b, *,} ,
Rui Wang ^c ,
Wenjie Zhou ^a ,
Sisi Zhou ^b ,
Yang Sun ^{d, *,} ,
Shuai Li ^{a, *,} ,
Zhaoxiang Wang ^e

a.
Department of Physics, Department of Materials Science and Engineering, and Institute for Applied Optics and Precision Engineering, Southern University of Science and Technology, Shenzhen 518055, China
b.
Wuhan Institute of Marine Electric Propulsion, Wuhan 430064, China
c.
Faculty of Materials Science and Chemistry, China University of Geosciences, Wuhan 430074, China
d.
School of Materials, Shenzhen Campus of Sun Yat-sen University, Shenzhen 518107, China
e.
Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, College of Materials Science and Optoelectronic Technology, University of Chinese Academy of Sciences, Beijing 100190, China

155212276@qq.com

sunyang5@mail.sysu.edu.cn

lis6@sustech.edu.cn

Received Date: 16 October 2024
Revised Date: 16 November 2024
Accepted Date: 26 November 2024
Available Online: 27 November 2024

Figures(7)

Anti-perovskite cathodes, typified by Li₂FeSO, hold great promise for Li-ion batteries due to their high specific capacity, cost-effectiveness, and ease of production. However, their utilization in high-energy-density batteries is hindered by low Li intercalation voltage and limited rate performance. This study employs first-principles calculations to assess the impact of element substitutions and doping on the voltage and Li-ion migration energy barrier in Li₂TMSO (TM = Cu, Ni, Co, Fe, V, Cr, Ti) anti-perovskite materials. Our findings reveal that replacing the S element with Se or Te in Li₂FeSO and Li₂MnSO can reduce the voltage. For Li₂TMSO (TM = Cu, Ni, Co, Fe, V, Cr, Ti), the voltage increases as TM changes from Ti to Ni. This process closely related to the downward shift of the TM-3d electron orbital energy level. When the energy level difference between TM-3d and S-3p orbital energy levels is large, the voltage is determined by TM-3d orbitals. When the difference is small, S-3p participates in the reaction. Additionally, doping with the inactive element Mg could allow deeper energy level electrons to participate in the reaction, thus increasing the voltage. To simultaneously enhance intercalation voltage and rate performance, we investigated multi-element doping strategies for anti-perovskite cathode materials. Our study establishes a solid foundation the development of high-voltage anti-perovskite cathodes, holding promise for significant advancements in energy storage technology.
- Cathodes materials,
- Anti-perovskite,
- Electron orbital energy level,
- Anionic redox,
- Li-ion transport
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