A gradient oxy-thiophosphate-coated Ni-rich layered oxide cathode for stable all-solid-state Li-ion batteries

Jianwen Liang; Yuanmin Zhu; Xiaona Li; Jing Luo; Sixu Deng; Yang Zhao; Yipeng Sun; Duojie Wu; Yongfeng Hu; Weihan Li; Tsun-Kong Sham; Ruying Li; Meng Gu; Xueliang Sun

doi:10.1038/s41467-022-35667-7

A gradient oxy-thiophosphate-coated Ni-rich layered oxide cathode for stable all-solid-state Li-ion batteries

Nat Commun. 2023 Jan 10;14(1):146. doi: 10.1038/s41467-022-35667-7.

Authors

Jianwen Liang^#¹, Yuanmin Zhu^#^{2

3}, Xiaona Li^#¹, Jing Luo¹, Sixu Deng¹, Yang Zhao¹, Yipeng Sun¹, Duojie Wu³, Yongfeng Hu⁴, Weihan Li^{1

5}, Tsun-Kong Sham⁵, Ruying Li¹, Meng Gu⁶, Xueliang Sun⁷

Affiliations

¹ Department of Mechanical and Materials Engineering, University of Western Ontario, London, ON, N6A 5B9, Canada.
² Research Institute of Interdisciplinary Science & School of Material Science and Engineering, Dongguan university of technology, Dongguan, Guangzhou, China.
³ Department of Materials Science and Engineering, Southern University of Science and Technology, Shenzhen, 518055, China.
⁴ Canadian Light Source, 44 Innovation Boulevard, Saskatoon, SK, S7N 2V3, Canada.
⁵ Department of Chemistry, University of Western Ontario, London, ON, N6A 5B9, Canada.
⁶ Department of Materials Science and Engineering, Southern University of Science and Technology, Shenzhen, 518055, China. gum@sustech.edu.cn.
⁷ Department of Mechanical and Materials Engineering, University of Western Ontario, London, ON, N6A 5B9, Canada. xsun9@uwo.ca.

^# Contributed equally.

Abstract

High-energy Ni-rich layered oxide cathode materials such as LiNi_0.8Mn_0.1Co_0.1O₂ (NMC811) suffer from detrimental side reactions and interfacial structural instability when coupled with sulfide solid-state electrolytes in all-solid-state lithium-based batteries. To circumvent this issue, here we propose a gradient coating of the NMC811 particles with lithium oxy-thiophosphate (Li₃P_1+xO₄S_4x). Via atomic layer deposition of Li₃PO₄ and subsequent in situ formation of a gradient Li₃P_1+xO₄S_4x coating, a precise and conformal covering for NMC811 particles is obtained. The tailored surface structure and chemistry of NMC811 hinder the structural degradation associated with the layered-to-spinel transformation in the grain boundaries and effectively stabilize the cathode|solid electrolyte interface during cycling. Indeed, when tested in combination with an indium metal negative electrode and a Li₁₀GeP₂S₁₂ solid electrolyte, the gradient oxy-thiophosphate-coated NCM811-based positive electrode enables the delivery of a specific discharge capacity of 128 mAh/g after almost 250 cycles at 0.178 mA/cm² and 25 °C.