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Engineering molecular regulation for SiOx with long-term stable cycle and high Coulombic efficiency as lithium-ion battery anodes

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Abstract

In the current situation where the practical application of silicon anode materials encounters great challenges, silicon oxide (SiOx, 0 ≤ x ≤ 2) has attracted the attention of researchers due to its relatively small volume expansion, stable cycling performance, and low cost, which is possible to realize commercial applications earlier than silicon anode. However, it remains a challenge to prepare SiOx materials with long-term stable cycling performance and high Coulombic efficiency using low-cost methods. In this work, SiOx anode material with high Coulombic efficiency and good long-term cycling stability was prepared at a low cost by hydrolysis of siloxane and in situ polymerization of phenolic resin. The hydrolysis of siloxane was further regulated by different silane coupling agents to regulate the size and microstructure of prepared SiOx materials, which displayed the substantially improved electrochemical performance. The excellent electrochemical performance of SiOx prepared by regulated hydrolysis of siloxane with silane coupling agents is attributed to the effect of silane coupling agent on size and microstructure of SiOx, revealing that the strategy of modulating the hydrolysis of siloxane by silane coupling agent is a potential method to prepare high-performance SiOx materials.

摘要

在硅负极材料实际应用面临巨大挑战的现状下, 氧化硅材料 (SiOx, 0 ≤ x ≤ 2) 由于其体积膨胀相对较小、循环性能稳定、成本较低, 有可能比硅负极更早实现商业应用, 受到研究人员的广泛关注。然而, 利用低成本的方法制备具有长期稳定循环性能和高库仑效率的SiOx材料仍然是一个挑战。本工作通过硅氧烷水解和酚醛树脂原位聚合, 以较低的成本制备了库仑效率高、长期循环稳定性好的SiOx负极材料。通过不同的硅烷偶联剂进一步调节硅氧烷的水解, 调控制备的SiOx材料的尺寸和微观结构, 从而显著提高了SiOx材料的电化学性能。硅烷偶联剂调控硅氧烷水解制备的SiOx具有优异的电化学性能, 归功于硅烷偶联剂对SiOx的尺寸和微观结构的影响, 揭示了一种利用硅烷偶联剂调控硅氧烷水解制备高性能SiOx材料的新方法。

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Acknowledgements

This study was financially supported by the National Natural Science Foundation of China (No. 22204159), the Instrument Developing Project of the Chinese Academy of Sciences (No. YJKYYQ20210003) and Natural Science Foundation of Jilin Province (No. 20210101402JC)

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Authors and Affiliations

  1. State Key Laboratory of Electroanalytical Chemistry, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun, 130022, China

    Fei Wang, Han Gao, Zhao-Yu Niu, Yao-Peng Zheng, Ming-Yan Chuai & Jia-Nan Xu

  2. University of Science and Technology of China, Hefei, 230026, China

    Han Gao

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  1. Fei Wang
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Wang, F., Gao, H., Niu, ZY. et al. Engineering molecular regulation for SiOx with long-term stable cycle and high Coulombic efficiency as lithium-ion battery anodes. Rare Met. 43, 588–598 (2024). https://doi.org/10.1007/s12598-023-02463-1

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