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Research Article

LiOH-mediated crystallization regulating strategy enhancing electrochemical performance and structural stability of SiO anodes for lithium-ion batteries

Zhengqiu He1, Zewen Xu1, Yu Long2, Jiexin Zhu3, Hao Yang1, Kuo Chen1, Qiang Zhou1, Ning Cao1, Xiaobo Wang1, Juan Wang1, Xiaojie Tan1, Litao Wang4, Luhai Wang4, Shengbao He4, Mengdi Zhang1(), Han Hu1, Mingbo Wu1 ()
State Key Laboratory of Heavy Oil Processing, College of Chemistry and Chemical Engineering, China University of Petroleum (East China), Qingdao 266580, China
Department of Chemistry, National University of Singapore, 3 Science Drive 3, Singapore 117543, Singapore
School of Chemical Sciences, University of Auckland, Auckland 1010, New Zealand
Petrochemical Research Institute, Petro China Company Ltd., Beijing 102206, China
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Graphical Abstract

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We introduce a novel method to precisely regulate the crystallization of SiO. Our findings establish a clear correlation between crystallinity and its electrochemical performance. Furthermore, we demonstrate that an optimal concentration of LiOH effectively inhibits the inward diffusion of oxygen atoms at the SiO surface. This interaction fosters the formation of a thin, oxygen-rich layer on the surface effectively reducing volumetric expansion during electrochemical reactions. The presence of this layer substantially enhances the material’s electrochemical performance. This structural substantially reduces volumetric expansion and enhances the electrochemical performance of the material.

Abstract

Silicon monoxide (SiO) is widely recognized as a promising anode material for next-generation lithium-ion batteries. Owing to its metastable amorphous structure, SiO exhibits a highly complex degree of crystallization at the microscopic level, which significantly influences its electrochemical behavior. As a consequence, accurately regulating the crystallization of SiO, and further establishing the relationship between crystallinity and electrochemical performance are very critical for SiO anodes. In this article, carbon-coated SiO materials with different crystallinity degrees were synthesized using lithium hydroxide monohydrate (LiOH·H2O) as a structural modifier to reveal this rule. Additionally, moderate amount of LiOH·H2O addition results in the forming of an oxygen-rich shell, which effectively inhibits the inward migration of oxygen atoms on the SiO surface and suppresses volume expansion. However, the crystallinity of SiO will gradually enhance and the crystalline phase appears with increasing the amount of LiOH·H2O, which will generate a deteriorative Li+ diffusion kinetic. After balancing the above two contradictions, a mass fraction of 1% LiOH·H2O for the additive yielded SiO@C-1, characterized by optimal crystallinity. SiO@C-1 demonstrates exceptional long-cycle stability with 74.8% capacity retention after 500 cycles at 1 A·g−1. Furthermore, it achieves a capacity retention of 52.2% even at a high density of 5 A·g−1. This study first reveals the relationship between SiO crystallinity and electrochemical performance, which efficiently guides the design of high-performance SiO anodes.

Keywords

lithium-ion batteriesSiO anodescrystallinity regulationhigh ratelong life

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Nano Research
Volume 17 Issue 9,
September 2024
Pages 8174-8183
DOI: 10.1007/s12274-024-6866-0
Cite this article:
He Z, Xu Z, Long Y, et al. LiOH-mediated crystallization regulating strategy enhancing electrochemical performance and structural stability of SiO anodes for lithium-ion batteries. Nano Research, 2024, 17(9): 8174-8183. https://doi.org/10.1007/s12274-024-6866-0
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