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 () and Xueliang Sun ()
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Jianwen Liang: University of Western Ontario
Yuanmin Zhu: Dongguan university of technology
Xiaona Li: University of Western Ontario
Jing Luo: University of Western Ontario
Sixu Deng: University of Western Ontario
Yang Zhao: University of Western Ontario
Yipeng Sun: University of Western Ontario
Duojie Wu: Southern University of Science and Technology
Yongfeng Hu: Canadian Light Source, 44 Innovation Boulevard
Weihan Li: University of Western Ontario
Tsun-Kong Sham: University of Western Ontario
Ruying Li: University of Western Ontario
Meng Gu: Southern University of Science and Technology
Xueliang Sun: University of Western Ontario

Nature Communications, 2023, vol. 14, issue 1, 1-12

Abstract: Abstract High-energy Ni-rich layered oxide cathode materials such as LiNi0.8Mn0.1Co0.1O2 (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 (Li3P1+xO4S4x). Via atomic layer deposition of Li3PO4 and subsequent in situ formation of a gradient Li3P1+xO4S4x 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.

Date: 2023
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DOI: 10.1038/s41467-022-35667-7

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