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Research Article

Stabilization of high-voltage layered oxide cathode by utilizing residual lithium to form NASICON-type nanoscale functional coating

Yabin Shen1,2Yingqiang Wu5Dongyu Zhang1,2Yao Liang1,2Dongming Yin1,2Limin Wang1,2Licheng Wang3( )Jingchao Cao4( )Yong Cheng1 ( )
State Key Laboratory of Rare Earth Resource Utilization, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun 130022, China
School of Applied Chemistry and Engineering, University of Science and Technology of China (USTC), Hefei 230026, China
College of Physics Science and Technology, Yangzhou University, Yangzhou 225002, China
Changsha Research Institute of Mining and Metallurgy Co., Ltd, Changsha 410012, China
Institute of Nuclear and New Energy Technology, Tsinghua University, Beijing 100084, China
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Abstract

High-voltage medium-nickel low-cobalt lithium layered oxide cathode materials are becoming a popular development route for high-energy lithium-ion batteries due to their relatively high capacity, low cost, and improved safety. Unfortunately, capacity fading derived from surface lithium residue, electrode-electrolyte interfacial side reactions, and bulk structure degradation severely limits large-scale commercial utilization. In this work, an ultrathin and uniform NASICON-type Li3V2(PO4)3 (LVP) nanoscale functional coating is formed in situ by utilizing residual lithium to enhance the lithium storage performance of LiNi0.6Co0.05Mn0.35O2 (NCM) cathode. The GITT and ex-situ EIS and XPS demonstrate exceptional Li+ diffusion and conductivity and attenuated interfacial side reactions, improving the electrode-electrolyte interface stability. The variable temperature in-situ XRD demonstrates delayed phase transition temperature to improve thermal stability. The battery in-situ XRD displays the single-phase H1-H2 reaction and weakened harmful H3 phase transition, minimizing the bulk mechanical degradation. These improvements are attributed to the removal of surface residual lithium and the formation of NASICON-type Li3V2(PO4)3 functional coatings with stable structure and high ionic and electronic conductivity. Consequently, the obtained NCM@LVP delivers a higher capacity retention rate (97.1% vs. 79.6%) after 150 cycles and a superior rate capacity (87 mAh·g–1 vs. 58 mAh·g–1) at a 5 C current density than the pristine NCM under a high cut-off voltage of 4.5 V. This work suggests a clever way to utilize residual lithium to form functional coatings in situ to improve the lithium storage performance of high-voltage medium-nickel low-cobalt cathode materials.

Graphical Abstract

An ultrathin and uniform NASICON-type Li3V2(PO4)3 nanoscale functional coating is formed in situ by utilizing residual lithium to enhance the lithium storage performance of high-voltage medium-nickel low-cobalt LiNi0.6Co0.05Mn0.35O2 cathode. Li3V2(PO4)3 functional coating improves electrode-electrolyte interfacial stability and bulk structural stability by eliminating residual lithium, preventing HF corrosion, inhibiting electrolyte decomposition, enhancing electronic/ionic conductivity, inhibiting transition metal dissolution, and attenuating microcrack formation.

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Nano Research
Pages 5973-5982

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Cite this article:
Shen Y, Wu Y, Zhang D, et al. Stabilization of high-voltage layered oxide cathode by utilizing residual lithium to form NASICON-type nanoscale functional coating. Nano Research, 2023, 16(4): 5973-5982. https://doi.org/10.1007/s12274-022-5298-y
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Received: 20 September 2022
Revised: 27 October 2022
Accepted: 05 November 2022
Published: 29 November 2022
© Tsinghua University Press 2022