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. Herein, 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. Furthermore, 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.
Hasa, Ivana, et al. "Electrochemical Reactivity and Passivation of Silicon Thin-Film Electrodes in Organic Carbonate Electrolytes." ACS Applied Materials and Interfaces, vol. 12, no. 36, Aug. 2020. https://doi.org/10.1021/acsami.0c09384
Hasa, Ivana, Haregewoin, Atetegeb M., Zhang, Liang, Tsai, Wan-Yu, Guo, Jinghua, Veith, Gabriel M., Ross, Philip N., & Kostecki, Robert (2020). Electrochemical Reactivity and Passivation of Silicon Thin-Film Electrodes in Organic Carbonate Electrolytes. ACS Applied Materials and Interfaces, 12(36). https://doi.org/10.1021/acsami.0c09384
@article{osti_1665998,
author = {Hasa, Ivana and Haregewoin, Atetegeb M. and Zhang, Liang and Tsai, Wan-Yu and Guo, Jinghua and Veith, Gabriel M. and Ross, Philip N. and Kostecki, Robert},
title = {Electrochemical Reactivity and Passivation of Silicon Thin-Film Electrodes in Organic Carbonate Electrolytes},
annote = {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. Herein, 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. Furthermore, 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.},
doi = {10.1021/acsami.0c09384},
url = {https://www.osti.gov/biblio/1665998},
journal = {ACS Applied Materials and Interfaces},
issn = {ISSN 1944-8244},
number = {36},
volume = {12},
place = {United States},
publisher = {American Chemical Society (ACS)},
year = {2020},
month = {08}}
Philosophical Transactions of the Royal Society of London. Series A: Mathematical, Physical and Engineering Sciences, Vol. 362, Issue 1817https://doi.org/10.1098/rsta.2003.1347