Nano-FTIR Spectroscopy of the Solid Electrolyte Interphase Layer on a Thin-Film Silicon Li-Ion Anode
Abstract
Si anodes for Li-ion batteries are notorious for their large volume expansion during lithiation and the corresponding detrimental effects on cycle life. However, calendar life is the primary roadblock for widespread adoption. During calendar life aging, the main origin of impedance increase and capacity fade is attributed to the instability of the solid electrolyte interphase (SEI). In this work, we use ex situ nano-Fourier transform infrared spectroscopy and X-ray photoelectron spectroscopy to characterize the structure and composition of the SEI layer on amorphous Si thin films after an accelerated calendar aging protocol. The characterization of the SEI on non-washed and washed electrodes shows that brief washing in dimethyl carbonate results in large changes to the film chemistry and topography. Detailed examination of the non-washed electrodes during the first lithiation and after an accelerated calendar aging protocol reveals that PF6– and its decomposition products tend to accumulate in the SEI due to the preferential transport of PF6– ions through polyethylene oxide-like species in the organic part of the SEI layer. This work demonstrates the importance of evaluating the SEI layer in its intrinsic, undisturbed form and new strategies to improve the passivation of the SEI layer are proposed.
- Authors:
-
[1];
[1];
- Energy Storage and Distributed Resources Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States
- Energy Storage and Distributed Resources Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States, Department of Mechanical Engineering, University of California, Berkeley, California 94720, United States
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Molecular Foundry
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO)
- OSTI Identifier:
- 1922120
- Alternate Identifier(s):
- OSTI ID: 2234177
- Grant/Contract Number:
- AC02-05CH11231
- Resource Type:
- Published Article
- Journal Name:
- ACS Applied Materials and Interfaces
- Additional Journal Information:
- Journal Name: ACS Applied Materials and Interfaces Journal Volume: 15 Journal Issue: 5; Journal ID: ISSN 1944-8244
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE; silicon; anode; SEI; electrolyte; interface; FTIR; spectroscopy; electrodes; electrolytes; infrared light; layers; surface chemistry
Citation Formats
Dopilka, Andrew, Gu, Yueran, Larson, Jonathan M., Zorba, Vassilia, and Kostecki, Robert. Nano-FTIR Spectroscopy of the Solid Electrolyte Interphase Layer on a Thin-Film Silicon Li-Ion Anode. United States: N. p., 2023.
Web. doi:10.1021/acsami.2c19484.
Dopilka, Andrew, Gu, Yueran, Larson, Jonathan M., Zorba, Vassilia, & Kostecki, Robert. Nano-FTIR Spectroscopy of the Solid Electrolyte Interphase Layer on a Thin-Film Silicon Li-Ion Anode. United States. https://doi.org/10.1021/acsami.2c19484
Dopilka, Andrew, Gu, Yueran, Larson, Jonathan M., Zorba, Vassilia, and Kostecki, Robert. Wed .
"Nano-FTIR Spectroscopy of the Solid Electrolyte Interphase Layer on a Thin-Film Silicon Li-Ion Anode". United States. https://doi.org/10.1021/acsami.2c19484.
@article{osti_1922120,
title = {Nano-FTIR Spectroscopy of the Solid Electrolyte Interphase Layer on a Thin-Film Silicon Li-Ion Anode},
author = {Dopilka, Andrew and Gu, Yueran and Larson, Jonathan M. and Zorba, Vassilia and Kostecki, Robert},
abstractNote = {Si anodes for Li-ion batteries are notorious for their large volume expansion during lithiation and the corresponding detrimental effects on cycle life. However, calendar life is the primary roadblock for widespread adoption. During calendar life aging, the main origin of impedance increase and capacity fade is attributed to the instability of the solid electrolyte interphase (SEI). In this work, we use ex situ nano-Fourier transform infrared spectroscopy and X-ray photoelectron spectroscopy to characterize the structure and composition of the SEI layer on amorphous Si thin films after an accelerated calendar aging protocol. The characterization of the SEI on non-washed and washed electrodes shows that brief washing in dimethyl carbonate results in large changes to the film chemistry and topography. Detailed examination of the non-washed electrodes during the first lithiation and after an accelerated calendar aging protocol reveals that PF6– and its decomposition products tend to accumulate in the SEI due to the preferential transport of PF6– ions through polyethylene oxide-like species in the organic part of the SEI layer. This work demonstrates the importance of evaluating the SEI layer in its intrinsic, undisturbed form and new strategies to improve the passivation of the SEI layer are proposed.},
doi = {10.1021/acsami.2c19484},
journal = {ACS Applied Materials and Interfaces},
number = 5,
volume = 15,
place = {United States},
year = {Wed Jan 25 00:00:00 EST 2023},
month = {Wed Jan 25 00:00:00 EST 2023}
}
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