Modulating the Surface Ligand Orientation for Stabilized Anionic Redox in Li‐Rich Oxide Cathodes

Liu, Yanchen; Zhu, He; Zhu, Hekang; Ren, Yang; Zhu, Yizhou; Huang, Yalan; Dai, Liang; Dou, Shuming; Xu, Jie; Sun, Cheng‐Jun; Wang, Xun‐Li; Deng, Yida; Yuan, Qunhui; Liu, Xingjun; Wu, Junwei; Chen, Yanan; Liu, Qi

doi:10.1002/aenm.202003479

Modulating the Surface Ligand Orientation for Stabilized Anionic Redox in Li‐Rich Oxide Cathodes

Journal Article · Tue Mar 02 23:00:00 EST 2021 · Advanced Energy Materials

DOI:https://doi.org/10.1002/aenm.202003479· OSTI ID:1804575

Liu, Yanchen ^[1]; Zhu, He ^[2]; Zhu, Hekang ^[2]; Ren, Yang ^[3]; Zhu, Yizhou ^[4]; Huang, Yalan ^[2]; Dai, Liang ^[2]; Dou, Shuming ^[5]; Xu, Jie ^[5]; Sun, Cheng‐Jun ^[3]; Wang, Xun‐Li ^[6]; Deng, Yida ^[5]; Yuan, Qunhui ^[7]; Liu, Xingjun ^[7]; Wu, Junwei ^[7]; ^[5]; Liu, Qi ^[6]

Shenzhen Key Laboratory of Advanced Materials Department of Materials Science and Engineering Harbin Institute of Technology (Shenzhen) Shenzhen 518055 P. R. China, School of Materials Science and Engineering Key Laboratory of Advanced Ceramics and Machining Technology of Ministry of Education Tianjin Key Laboratory of Composite and Functional Materials Tianjin University Tianjin 300072 P. R. China
Department of Physics City University of Hong Kong Hong Kong 999077 P. R. China
Argonne National Laboratory X‐Ray Science Division Argonne IL 60439 USA
Department of Materials Science and Engineering Northwestern University Argonne IL 0201 USA
School of Materials Science and Engineering Key Laboratory of Advanced Ceramics and Machining Technology of Ministry of Education Tianjin Key Laboratory of Composite and Functional Materials Tianjin University Tianjin 300072 P. R. China
Department of Physics City University of Hong Kong Hong Kong 999077 P. R. China, Shenzhen Research Institute City University of Hong Kong Shenzhen 518057 P. R. China
Shenzhen Key Laboratory of Advanced Materials Department of Materials Science and Engineering Harbin Institute of Technology (Shenzhen) Shenzhen 518055 P. R. China

Abstract

Anionic redox chemistry is emerging as a key concept in the development of high‐energy lithium‐ion batteries, as it enables a nearly doubled charge storage capacity, aiding the development of high‐capacity batteries. However, the anionic reactivity is frequently irreversible from charge to discharge, leading to rapid decay of the capacity and voltage of batteries over long‐term cycling. Although the possibility of controlling the anionic redox reactions by tuning the geometric and electronic structures has recently been proposed, the implementation of this strategy is still a critical challenge. Herein, a strategy is proposed to improve the anionic redox reversibility of a model anionic redox active cathode material, Li _1.2 Ni _0.13 Co _0.13 Mn _0.54 O ₂ , by tuning the surface ligand geometry via the growth of a lattice‐compatible spinel LiCoO ₂ coating layer on the particle surface. Detailed local structure and first principles investigations reveal that the shape and orientation of the octahedral layer in the host lattice are modified. Accordingly, a two‐band oxygen redox behavior is triggered in the ligand‐orientation‐regulated Li‐rich cathode, leading to enhanced reversibility, and thus, remarkably improved capacity and voltage retention over cycling. This study highlights the importance of controllable ligand orientation, carving a new path for the development and design of Li‐rich cathodes in the future.

View Accepted Manuscript (Publisher)

Sponsoring Organization:: USDOE

Grant/Contract Number:: NONE; AC02-06CH11357

OSTI ID:: 1804575

Alternate ID(s):: OSTI ID: 23098885

Journal Information:: Advanced Energy Materials, Journal Name: Advanced Energy Materials Journal Issue: 13 Vol. 11; ISSN 1614-6832

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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