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DOE OSTI · 2570562

Entropy-Tailored Fast-Charging Sodium Layered Cathodes

Wang, Haoji [Central South University, Changsha (China)]·Mei, Yu [Central South University, Changsha (China); Argonne National Laboratory (ANL), Argonne, IL (United States)]·Gao, Jinqiang [Central South University, Changsha (China)]·Ni, Lianshan [Central South University, Changsha (China)]·Hong, Ningyun [Central South University, Changsha (China)]·Ma, Lu [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)]·Kwon, Gihan [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)] (ORCID:0000000279632136)·Huang, Jiangnan [Central South University, Changsha (China)]·He, Yi [Central South University, Changsha (China)]·Deng, Wentao [Central South University, Changsha (China)]·Zou, Guoqiang [Central South University, Changsha (China)]·Hou, Hongshuai [Central South University, Changsha (China)] (ORCID:0000000182014614)·Liang, Chaoping [Central South University, Changsha (China)] (ORCID:0000000229102938)·Liu, Tongchao [Argonne National Laboratory (ANL), Argonne, IL (United States)] (ORCID:0000000260103891)·Ji, Xiaobo [Central South University, Changsha (China)] (ORCID:0000000254057913)·Amine, Khalil [Argonne National Laboratory (ANL), Argonne, IL (United States); Univ. of Chicago, IL (United States)] (ORCID:0000000192063719)
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Abstract

O3-type layered transition metal (TM) oxides are widely used as cathode materials for Na-ion batteries due to their high energy density potential, enabled by the state of charge (SoC)-dependent transition from octahedral (O-type) to prismatic (P-type) structures during Na-ion (de)sodiation. However, the O–P transition is often criticized for compromising the Na-ion mobility and limiting the cycle life. Herein, we reveal the intrinsic correlation between O–P transitions, oxygen behaviors, and Na-ion kinetics. We demonstrate that a compositionally versatile, entropy-tailored approach can promote preferred transitions (characterized by large lattice parameter deviations in the O-type region and rapid O–P biphasic reactions), enhancing Na-ion migration, as revealed by in situ high-energy synchrotron X-ray diffraction (HEXRD). Additionally, irreversible oxygen loss at high SoC is effectively mitigated, while TM migration and surface reconstruction are greatly suppressed, further accelerating Na-ion transport and stabilizing the structure, as confirmed by X-ray absorption spectroscopy (XAS) and theoretical analyses. The result is an exceptionally high rate capability of 88.7 mAh g –1 at 20 C (2.4 A g –1 ) with a superior normalized retention of 72.6%, accompanied by a prolonged lifetime with 74.3% retention after 1000 cycles. In conclusion, this work advances the understanding of the chemistry–property relationships in O3-type layered cathodes and broadens the prospects for fabricating high-power-density electrodes.

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36 MATERIALS SCIENCEFast chargingMitigated oxygen lossNa-ion mobilityPreferred transitionSodium layered cathodes

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Wang, Haoji [Central South University, Changsha (China)], Mei, Yu [Central South University, Changsha (China); Argonne National Laboratory (ANL), Argonne, IL (United States)], Gao, Jinqiang [Central South University, Changsha (China)], Ni, Lianshan [Central South University, Changsha (China)], Hong, Ningyun [Central South University, Changsha (China)], Ma, Lu [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)], Kwon, Gihan [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)] (ORCID:0000000279632136), Huang, Jiangnan [Central South University, Changsha (China)], He, Yi [Central South University, Changsha (China)], Deng, Wentao [Central South University, Changsha (China)], Zou, Guoqiang [Central South University, Changsha (China)], Hou, Hongshuai [Central South University, Changsha (China)] (ORCID:0000000182014614), Liang, Chaoping [Central South University, Changsha (China)] (ORCID:0000000229102938), Liu, Tongchao [Argonne National Laboratory (ANL), Argonne, IL (United States)] (ORCID:0000000260103891), Ji, Xiaobo [Central South University, Changsha (China)] (ORCID:0000000254057913), Amine, Khalil [Argonne National Laboratory (ANL), Argonne, IL (United States); Univ. of Chicago, IL (United States)] (ORCID:0000000192063719). 2025-02-03. Entropy-Tailored Fast-Charging Sodium Layered Cathodes. https://doi.org/10.1021/jacs.4c12733

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36 MATERIALS SCIENCE↗