LiMnO2 cathode stabilized by interfacial orbital ordering for sustainable lithium-ion batteries

Xiaohui Zhu, Fanqi Meng, Qinghua Zhang, Liang Xue, He Zhu, Si Lan, Qi Liu (), Jing Zhao, Yuhang Zhuang, Qiubo Guo, Bo Liu, Lin Gu (), Xia Lu, Yang Ren and Hui Xia ()
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Xiaohui Zhu: Nanjing University of Science and Technology
Fanqi Meng: Chinese Academy of Sciences
Qinghua Zhang: Chinese Academy of Sciences
Liang Xue: Nanjing University of Science and Technology
He Zhu: City University of Hong Kong
Si Lan: Nanjing University of Science and Technology
Qi Liu: City University of Hong Kong
Jing Zhao: Nanjing University of Science and Technology
Yuhang Zhuang: Nanjing University of Science and Technology
Qiubo Guo: Nanjing University of Science and Technology
Bo Liu: Nanjing University of Science and Technology
Lin Gu: Chinese Academy of Sciences
Xia Lu: Sun Yat-Sen University
Yang Ren: Argonne National Laboratory
Hui Xia: Nanjing University of Science and Technology

Nature Sustainability, 2021, vol. 4, issue 5, 392-401

Abstract: Abstract Global lithium-ion battery deployments stand poised to grow substantially in the coming years, but it will be necessary to include sustainability considerations in the design of electrode materials. The current cathode chemistry relies heavily on cobalt, which, due to its scarcity and the environmental abuse and violation of human rights during its mining, must be replaced by abundant and environmentally friendly elements such as redox-active manganese. LiMnO2 is a strong contender for sustainable cathodes but cycles poorly because the Jahn–Teller distorted Mn3+ ions destabilize the lattice framework. Here, we report a LiMnO2 cathode design with interwoven spinel and layered domains. At the interface between these two domains, the Mn dz2 orbitals are oriented perpendicular to each other, giving rise to interfacial orbital ordering, which suppresses the otherwise cooperative Jahn–Teller distortion and Mn dissolution. As a result, the heterostructured cathode delivers enhanced structural and electrochemical cycling stability. This work provides a new strategy for interface engineering, possibly stimulating more research on Mn-rich cathode materials for sustainable lithium-ion batteries.

Date: 2021
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DOI: 10.1038/s41893-020-00660-9

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