Slight Multielement Doping-Induced Structural Order-Disorder Transition for High-Performance Layered Na-Ion Oxide Cathodes

Slight Multielement Doping-Induced Structural Order-Disorder Transition for High-Performance Layered Na-Ion Oxide Cathodes

Guo, Hao (China Institute of Atomic Energy)
Zhao, C. (TU Delft RST/Storage of Electrochemical Energy)
Gao, Jianxiang (China Institute of Atomic Energy)
Yang, Wenyun (Peking University)
Hu, Xufeng (China Institute of Atomic Energy)
Ma, Xiaobai (China Institute of Atomic Energy)
Jiao, Xuesheng (China Institute of Atomic Energy)
Yang, Jinbo (Peking University)
Sun, Kai (China Institute of Atomic Energy)
Chen, Dongfeng (China Institute of Atomic Energy)

2023

To realize concurrently the high-energy density and excellent cycling stability, maximum utilization of redox couple, minimization of detrimental phase transition, and structural degradation of O3-type layered oxide cathodes are critical for developing Na-ion batteries. Ni²⁺/Ni⁴⁺ redox couple showing multielectron reaction and higher redox potential is favorable to increase the energy density. However, the Jahn-Teller distortion of Ni³⁺ generated upon (dis)charging results in a strong anisotropy in the local crystal structure that causes irreversible interlayer bending and chemo-mechanical cracks of the cathode particles, compromising the electrochemical properties eventually. In this work, we show a slight multielement doping strategy that enlarges the amount of active redox components while minimizing the inactive contents. The results show that the uniform distribution of multiple components can help increase the disorder degree of atom arrangement and alleviate the structural changes and detrimental anisotropy cracks. As a proof of concept, a multielement-doped O3-type Na_0.9Ni_0.25Cu_0.05Mg_0.05Zn_0.05Fe_0.05Al_0.05Mn_0.40Ti_0.05Sn_0.05O₂ oxide is rationally prepared that presents better chemo-mechanical stability and delayed O3-P3 phase transition behavior. Compared to the high Ni-content Na_0.9Ni_0.35Fe_0.2Mn_0.45O₂ cathode, this as-prepared multielement material delivers a reversible capacity of about 120 mAh/g in the voltage range of 2-4.0 V, superior cycling stability with 90% of capacity retention after 500 cycles, and excellent rate capability (more than 70% of initial capacity at 5.0 C). This work indicates that the multielement doping method is highly suitable for the development of advanced Na-ion layered oxide cathodes.

anisotropy lattice strain
multielement doping
NaNiCuMgZnFeAlMnTiSnO
O3-type
order−disorder transition

http://resolver.tudelft.nl/uuid:c584f05e-539c-4769-9b0a-8bc640296505

https://doi.org/10.1021/acsami.3c04843

2024-01-13

1944-8244

ACS applied materials & interfaces, 15 (29), 34789-34796

Green Open Access added to TU Delft Institutional Repository 'You share, we take care!' - Taverne project https://www.openaccess.nl/en/you-share-we-take-care Otherwise as indicated in the copyright section: the publisher is the copyright holder of this work and the author uses the Dutch legislation to make this work public.

Institutional Repository

journal article

© 2023 Hao Guo, C. Zhao, Jianxiang Gao, Wenyun Yang, Xufeng Hu, Xiaobai Ma, Xuesheng Jiao, Jinbo Yang, Kai Sun, Dongfeng Chen