Introducing 4s-2p Orbital Hybridization to Stabilize Spinel Oxide Cathodes for Lithium-Ion Batteries

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2022

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Liang, G.
Olsson, E.
Zou, J.
Wu, Z.
Li, J.
Lu, C.-Z.
D'Angelo, A.M.
Johannessen, B.
Thomsen, L.
Cowie, B.

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Angewandte Chemie International Edition, 2022; 61(27)

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Dr. Gemeng Liang, Dr. Emilia Olsson, Dr. Jinshuo Zou, Dr. Zhibin Wu, Jingxi Li, Dr. Cheng-Zhang Lu, Dr. Anita M. D'Angelo, Dr. Bernt Johannessen, Dr. Lars Thomsen, Dr. Bruce Cowie, Prof. Vanessa K. Peterson, Prof. Qiong Cai, Dr. Wei Kong Pang, Prof. Zaiping Guo

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Abstract

Oxides composed of an oxygen framework and interstitial cations are promising cathode materials for lithium-ion batteries. However, the instability of the oxygen framework under harsh operating conditions results in fast battery capacity decay, due to the weak orbital interactions between cations and oxygen (mainly 3d–2p interaction). Here, a robust and endurable oxygen framework is created by introducing strong 4s–2p orbital hybridization into the structure using LiNi0.5Mn1.5O4 oxide as an example. The modified oxide delivers extraordinarily stable battery performance, achieving 71.4 % capacity retention after 2000 cycles at 1 C. This work shows that an orbital-level understanding can be leveraged to engineer high structural stability of the anion oxygen framework of oxides. Moreover, the similarity of the oxygen lattice between oxide electrodes makes this approach extendable to other electrodes, with orbital-focused engineering a new avenue for the fundamental modification of battery materials.

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Published online 25 April 2022

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© 2022 The Authors. Angewandte Chemie International Edition published by Wiley-VCHGmbH.This is an open access article under the terms of the Creative Commons Attribution Non-Commercial NoDerivs License ,which permits use and distribution in any medium, provided the original work is properly cited,the use is non-commercial and no modifications or adaptations are made.

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