Tailoring chemical composition of solid electrolyte interphase by selective dissolution for long-life micron-sized silicon anode

Yi-Fan Tian, Shuang-Jie Tan, Chunpeng Yang, Yu-Ming Zhao, Di-Xin Xu, Zhuo-Ya Lu, Ge Li, Jin-Yi Li, Xu-Sheng Zhang, Chao-Hui Zhang, Jilin Tang, Yao Zhao, Fuyi Wang, Rui Wen, Quan Xu and Yu-Guo Guo ()
Additional contact information
Yi-Fan Tian: Institute of Chemistry Chinese Academy of Sciences (CAS)
Shuang-Jie Tan: Institute of Chemistry Chinese Academy of Sciences (CAS)
Chunpeng Yang: Tianjin University
Yu-Ming Zhao: Institute of Chemistry Chinese Academy of Sciences (CAS)
Di-Xin Xu: Institute of Chemistry Chinese Academy of Sciences (CAS)
Zhuo-Ya Lu: Institute of Chemistry Chinese Academy of Sciences (CAS)
Ge Li: Beijing IAmetal New Energy Technology Co., Ltd
Jin-Yi Li: Beijing IAmetal New Energy Technology Co., Ltd
Xu-Sheng Zhang: Institute of Chemistry Chinese Academy of Sciences (CAS)
Chao-Hui Zhang: Institute of Chemistry Chinese Academy of Sciences (CAS)
Jilin Tang: University of Chinese Academy of Sciences
Yao Zhao: University of Chinese Academy of Sciences
Fuyi Wang: University of Chinese Academy of Sciences
Rui Wen: Institute of Chemistry Chinese Academy of Sciences (CAS)
Quan Xu: Beijing IAmetal New Energy Technology Co., Ltd
Yu-Guo Guo: Institute of Chemistry Chinese Academy of Sciences (CAS)

Nature Communications, 2023, vol. 14, issue 1, 1-10

Abstract: Abstract Micron-sized Si anode promises a much higher theoretical capacity than the traditional graphite anode and more attractive application prospect compared to its nanoscale counterpart. However, its severe volume expansion during lithiation requires solid electrolyte interphase (SEI) with reinforced mechanical stability. Here, we propose a solvent-induced selective dissolution strategy to in situ regulate the mechanical properties of SEI. By introducing a high-donor-number solvent, gamma-butyrolactone, into conventional electrolytes, low-modulus components of the SEI, such as Li alkyl carbonates, can be selectively dissolved upon cycling, leaving a robust SEI mainly consisting of lithium fluoride and polycarbonates. With this strategy, raw micron-sized Si anode retains 87.5% capacity after 100 cycles at 0.5 C (1500 mA g−1, 25°C), which can be improved to >300 cycles with carbon-coated micron-sized Si anode. Furthermore, the Si||LiNi0.8Co0.1Mn0.1O2 battery using the raw micron-sized Si anode with the selectively dissolved SEI retains 83.7% capacity after 150 cycles at 0.5 C (90 mA g−1). The selective dissolution effect for tailoring the SEI, as well as the corresponding cycling life of the Si anodes, is positively related to the donor number of the solvents, which highlights designing high-donor-number electrolytes as a guideline to tailor the SEI for stabilizing volume-changing alloying-type anodes in high-energy rechargeable batteries.

Date: 2023
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DOI: 10.1038/s41467-023-43093-6

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