4.8 Article

Electrochemical Reactivity and Passivation of Silicon Thin-Film Electrodes in Organic Carbonate Electrolytes

期刊

ACS APPLIED MATERIALS & INTERFACES
卷 12, 期 36, 页码 40879-40890

出版社

AMER CHEMICAL SOC
DOI: 10.1021/acsami.0c09384

关键词

lithium-ion battery; silicon anode; solid electrolyte interphase (SEI); interfacial reactivity; passivation; thin film; lithium ethylene decarbonate; SEI breathing

资金

  1. Assistant Secretary for Energy Efficiency and Renewable Energy, Office of Vehicle Technologies of the U.S. Department of Energy under the Silicon Electrolyte Interface Stabilization (SEISta) Consortium [DE-AC02-05CH11231]
  2. DOE [DE-AC02-05CH11231]
  3. U.S. Department of Energy (DOE) [DE-AC05-00OR22725]

向作者/读者索取更多资源

This work focuses on the mechanisms of interfacial processes at the surface of amorphous silicon thin-film electrodes in organic carbonate electrolytes to unveil the origins of the inherent nonpassivating behavior of silicon anodes in Li-ion batteries. Attenuated total reflection Fourier-transform infrared spectroscopy, X-ray absorption spectroscopy, and infrared near-field scanning optical microscopy were used to investigate the formation, evolution, and chemical composition of the surface layer formed on Si upon cycling. We found that the chemical composition and thickness of the solid/electrolyte interphase (SEI) layer continuously change during the charging/discharging cycles. This SEI layer breathing effect is directly related to the formation of lithium ethylene dicarbonate (LiEDC) and LiPF6 salt decomposition products during silicon lithiation and their subsequent disappearance upon delithiation. The detected appearance and disappearance of LiEDC and LiPF6 decomposition compounds in the SEI layer are directly linked with the observed interfacial instability and poor passivating behavior of the silicon anode.

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