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

Hasa, Ivana; Haregewoin, Atetegeb M.; Zhang, Liang; Tsai, Wan-Yu; Guo, Jinghua; Veith, Gabriel M.; Ross, Philip N.; Kostecki, Robert

doi:10.1021/acsami.0c09384

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

Journal Article · Tue Aug 11 00:00:00 EDT 2020 · ACS Applied Materials and Interfaces

DOI:https://doi.org/10.1021/acsami.0c09384· OSTI ID:1665998

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^[4]; Ross, Philip N. ^[2]; Kostecki, Robert ^[2]

Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of Warwick, Coventry (United Kingdom)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

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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Research Organization:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE)

Grant/Contract Number:: AC05-00OR22725; AC02-05CH11231

OSTI ID:: 1665998

Alternate ID(s):: OSTI ID: 1775411

Journal Information:: ACS Applied Materials and Interfaces, Vol. 12, Issue 36; ISSN 1944-8244

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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