Non-topotactic reactions enable high rate capability in Li-rich cathode materials

Jianping Huang, Peichen Zhong, Yang Ha, Deok-Hwang Kwon, Matthew J. Crafton, Yaosen Tian, Mahalingam Balasubramanian, Bryan D. McCloskey, Wanli Yang and Gerbrand Ceder ()
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Jianping Huang: Lawrence Berkeley National Laboratory
Peichen Zhong: Lawrence Berkeley National Laboratory
Yang Ha: Lawrence Berkeley National Laboratory
Deok-Hwang Kwon: Lawrence Berkeley National Laboratory
Matthew J. Crafton: University of California Berkeley
Yaosen Tian: Lawrence Berkeley National Laboratory
Mahalingam Balasubramanian: Argonne National Laboratory
Bryan D. McCloskey: University of California Berkeley
Wanli Yang: Lawrence Berkeley National Laboratory
Gerbrand Ceder: Lawrence Berkeley National Laboratory

Nature Energy, 2021, vol. 6, issue 7, 706-714

Abstract: Abstract High-rate cathode materials for Li-ion batteries require fast Li transport kinetics, which typically rely on topotactic Li intercalation/de-intercalation because it minimally disrupts Li transport pathways. In contrast to this conventional view, here we demonstrate that the rate capability in a Li-rich cation-disordered rocksalt cathode can be significantly improved when the topotactic reaction is replaced by a non-topotactic reaction. The fast non-topotactic lithiation reaction is enabled by facile and reversible transition metal octahedral-to-tetrahedral migration, which improves rather than impedes Li transport. Using this concept, we show that high-rate performance can be achieved in Mn- and Ni-based cation-disordered rocksalt materials when some of the transition metal content can reversibly switch between octahedral and tetrahedral sites. This study provides a new perspective on the design of high-performance cathode materials by demonstrating how the interplay between Li and transition metal migration in materials can be conducive to fast non-topotactic Li intercalation/de-intercalations.

Date: 2021
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DOI: 10.1038/s41560-021-00817-6

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