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Nano Research 2023, 16(4): 5973-5982 https://doi.org/10.1007/s12274-022-5298-y
Research Article | Issue | Published: 29 November 2022

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

Show Author's Information Yabin Shen1,2,  Yingqiang Wu5,  Dongyu Zhang1,2,  Yao Liang1,2,  Dongming Yin1,2,  Limin Wang1,2,  Licheng 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
Keywords:
lithium-ion battery, surface modification, high-voltage medium-nickel low-cobalt cathode, residual lithium, NASICON-type Li3V2(PO4)3
Topics:
Synthesis
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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Abstract Full text Electronic supplementary material About this article

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.


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Electronic supplementary material
About this article

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

Show Author's information Yabin Shen1,2, Yingqiang Wu5, Dongyu Zhang1,2, Yao Liang1,2, Dongming Yin1,2, Limin Wang1,2, Licheng 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

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.

Keywords: lithium-ion battery, surface modification, high-voltage medium-nickel low-cobalt cathode, residual lithium, NASICON-type Li3V2(PO4)3

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Publication history
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Acknowledgements

Publication history

Received: 20 September 2022
Revised: 27 October 2022
Accepted: 05 November 2022
Published: 29 November 2022
Issue date: April 2023

Copyright

© Tsinghua University Press 2022

Acknowledgements

Acknowledgements

This research is funded by the National Key R&D Program of China (No. 2017YFE0198100), the National Natural Science Foundation of China (No. 21975250), the Key R&D Program of Jilin Province (No. 20220201132GX), the Key R&D Program of Hubei Province (No. 2022BAA084), and the Capital Construction Fund Projects within the Budget of Jilin Province (2021C037-2).

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