Multifunctional Integration of Double-Shell Hybrid Nanostructure for Alleviating Surface Degradation of LiNi0.8Co0.1Mn0.1O2 Cathode for Advanced Lithium-Ion Batteries at High Cutoff Voltage

Qiwen Ran; Hongyuan Zhao; Youzuo Hu; Shuai Hao; Qianqian Shen; Jintao Liu; Hao Li; Yu Xiao; Lei Li; Liping Wang; Xingquan Liu

doi:10.1021/acsami.9b20872

Multifunctional Integration of Double-Shell Hybrid Nanostructure for Alleviating Surface Degradation of LiNi_0.8Co_0.1Mn_0.1O₂ Cathode for Advanced Lithium-Ion Batteries at High Cutoff Voltage

ACS Appl Mater Interfaces. 2020 Feb 26;12(8):9268-9276. doi: 10.1021/acsami.9b20872. Epub 2020 Feb 17.

Authors

Qiwen Ran¹, Hongyuan Zhao^{1

2}, Youzuo Hu¹, Shuai Hao¹, Qianqian Shen³, Jintao Liu¹, Hao Li¹, Yu Xiao¹, Lei Li¹, Liping Wang¹, Xingquan Liu¹

Affiliations

¹ R&D Center for New Energy Materials and Integrated Energy Devices, School of Materials and Energy , University of Electronic Science and Technology of China , Chengdu 610054 , China.
² Research Center for Advanced Materials and Electrochemical Technology , Henan Institute of Science and Technology , Xinxiang 453003 , China.
³ College of Materials Science and Engineering , Sichuan University , Chengdu 610065 , China.

PMID: 32031362
DOI: 10.1021/acsami.9b20872

Abstract

Ni-rich LiNi_0.8Co_0.1Mn_0.1O₂ (NCM811) cathode is considered to be among the most promising candidates for high-energy-density lithium-ion batteries (LIBs). However, both capacity fading and structural degradation occur during long-term cycling, which extremely limit the commercial applications of NCM811, especially at a high cutoff voltage (>4.3 V). Here, we design a double-shell hybrid nanostructure consisting of a Li₂SiO₃ coating layer and a cation-mixed layer (Fm3̅m phase) to improve its electrochemical performance. Consequently, the Si-modified NCM811 electrode shows outstanding cycling stability with a 95.2% capacity retention at 4.3 V after 100 cycles and 87.3% at a 4.5 V high cutoff voltage after 100 cycles. This designed double-shell hybrid nanostructure alleviates side reactions, structural degradation, and internal cracking, effectively enhancing the surface structural stability. This efficient strategy provides a valuable step toward further commercial applications of the LiNi_0.8Co_0.1Mn_0.1O₂ cathode and enriches the fundamental understanding of layered cathode materials.

Keywords: LiNi0.8Co0.1Mn0.1O2; cycling stability; double-shell modification; hybrid nanostructure; structural degradation.