Electrochemical Reactivity and Passivation of Silicon Thin-Film Electrodes in Organic Carbonate Electrolytes
Abstract
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.
- Authors:
-
- 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)
- Publication Date:
- Research Org.:
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Energy Efficiency and Renewable Energy (EERE)
- OSTI Identifier:
- 1665998
- Alternate Identifier(s):
- OSTI ID: 1775411
- Grant/Contract Number:
- AC05-00OR22725; AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Applied Materials and Interfaces
- Additional Journal Information:
- Journal Volume: 12; Journal Issue: 36; Journal ID: ISSN 1944-8244
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE; lithium-ion battery; silicon anode; solid electrolyte interphase (SEI); interfacial reactivity; passivation; thin film; lithium ethylene
Citation Formats
Hasa, Ivana, Haregewoin, Atetegeb M., Zhang, Liang, Tsai, Wan-Yu, Guo, Jinghua, Veith, Gabriel M., Ross, Philip N., and Kostecki, Robert. Electrochemical Reactivity and Passivation of Silicon Thin-Film Electrodes in Organic Carbonate Electrolytes. United States: N. p., 2020.
Web. doi:10.1021/acsami.0c09384.
Hasa, Ivana, Haregewoin, Atetegeb M., Zhang, Liang, Tsai, Wan-Yu, Guo, Jinghua, Veith, Gabriel M., Ross, Philip N., & Kostecki, Robert. Electrochemical Reactivity and Passivation of Silicon Thin-Film Electrodes in Organic Carbonate Electrolytes. United States. 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., and Kostecki, Robert. Tue .
"Electrochemical Reactivity and Passivation of Silicon Thin-Film Electrodes in Organic Carbonate Electrolytes". United States. https://doi.org/10.1021/acsami.0c09384. https://www.osti.gov/servlets/purl/1665998.
@article{osti_1665998,
title = {Electrochemical Reactivity and Passivation of Silicon Thin-Film Electrodes in Organic Carbonate Electrolytes},
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},
abstractNote = {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.},
doi = {10.1021/acsami.0c09384},
journal = {ACS Applied Materials and Interfaces},
number = 36,
volume = 12,
place = {United States},
year = {Tue Aug 11 00:00:00 EDT 2020},
month = {Tue Aug 11 00:00:00 EDT 2020}
}
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