Issue 19, 2024

Thermodynamically stable low-Na O3 cathode materials driven by intrinsically high ionic potential discrepancy

Abstract

The thermodynamically stable window for an O3-type layered sodium cathode material is largely determined by its Na stoichiometry; a spontaneous transition to the P-type structure occurs when it is relatively low. With such limitation, the capacity and stability of O3-structured materials become restricted and a potentially promising class of O3-type materials that garner the structural stability of P2-type materials is underexplored. This work discovers that a large ionic potential discrepancy within the transition metal layer acts as a driving force that pushes the Na-ions from prismatic coordination to octahedral coordination. Utilizing this strategy, we have explored a class of off-stoichiometric O3-type materials with exceptionally low Na-stoichiometry (generally forming P2-type structures with higher thermodynamic stability) yet having the structural parameter features of P-type materials. These materials demonstrate rapid O3–P3 phase transition while maintaining a stable solid solution reaction at high voltages, resulting in an impressive P-phase range of 81.4%, thus showing superior performance compared with conventional O3-type materials. This principle provides a great extension to the existing family of layered cathode materials for sodium-ion batteries.

Graphical abstract: Thermodynamically stable low-Na O3 cathode materials driven by intrinsically high ionic potential discrepancy

Supplementary files

Article information

Article type
Paper
Submitted
30 May 2024
Accepted
07 Aug 2024
First published
22 Aug 2024

Energy Environ. Sci., 2024,17, 7058-7068

Thermodynamically stable low-Na O3 cathode materials driven by intrinsically high ionic potential discrepancy

M. Li, H. Zhuo, Y. Xu, Q. Jing, Y. Wu, Y. Gu, Z. Liao, K. Wang, M. Song, X. Li, J. Liang, C. Zhao, Y. Jiang, T. Wu, D. Geng, J. Hu, X. Sun and B. Xiao, Energy Environ. Sci., 2024, 17, 7058 DOI: 10.1039/D4EE02359E

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