Multicationic interactions mitigating lattice strain in sodium layered cathodes

Haoji Wang, Tongchao Liu (), Hongyi Chen, Yu Mei, Jinqiang Gao, Lianshan Ni, Ningyun Hong, Jiangnan Huang, Xinyu Hu, Wentao Deng, Guoqiang Zou, Hongshuai Hou, Debbie S. Silvester, Craig E. Banks, Xiaobo Ji () and Khalil Amine ()
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Haoji Wang: Central South University
Tongchao Liu: Argonne National Laboratory
Hongyi Chen: Central South University
Yu Mei: Central South University
Jinqiang Gao: Central South University
Lianshan Ni: Central South University
Ningyun Hong: Central South University
Jiangnan Huang: Central South University
Xinyu Hu: Central South University
Wentao Deng: Central South University
Guoqiang Zou: Central South University
Hongshuai Hou: Central South University
Debbie S. Silvester: Curtin University
Craig E. Banks: Manchester Metropolitan University
Xiaobo Ji: Central South University
Khalil Amine: Argonne National Laboratory

Nature Communications, 2025, vol. 16, issue 1, 1-13

Abstract: Abstract Transition-metal (TM) layered oxides have emerged as the primary cathode choice for sodium-ion batteries (SIBs) due to their high energy density and sustainable chemistry using non-critical elements. However, their anisotropic lattice strain and stress accumulation during (de)sodiation lead to severe structural degradation, yet an intrinsic strain-depressant approach remains elusive. Herein, we propose entropy regulation with zero Li/Co usage to mitigate harmful lattice displacements and enhance the electrochemical performance of sodium layered cathodes. Our findings demonstrate that high entropy design effectively inhibits TMO6 octahedra distortions upon cycling, as evidenced by hard X-ray absorption spectroscopy, greatly reducing near-surface structural deconstruction and interface side reactions. Furthermore, multicationic interactions driven by configurational entropy thermodynamically mitigate the formation of oxygen defects and strengthen ligand-to-metal coordination. The complementarity inherent in charge compensation within complex systems is unveiled and the restrained lattice parameters deviations without interior volume residuals are successfully achieved. As a result, the multicationic cathode exhibits improved cycling stability and Na+ diffusion kinetics in both half and full cells. The cathode chemistries outlined here broaden the prospects for lattice engineering to alleviate bulk fatigue and open up the possibility to develop an economically viable layered oxides with long durability.

Date: 2025
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DOI: 10.1038/s41467-025-59666-6

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