Chemistry of Electrolyte Reduction on Lithium Silicide
Abstract
Silicon anodes are promising for next-generation lithium-ion batteries due to high theoretical capacity. However, their performance and lifetime are currently limited by continuous electrolyte reduction and solid-electrolyte interphase (SEI) formation. Thus, SEI studies are important but often complicated due to the rough morphology of samples, buried interfaces, and the presence of binders. Here, we demonstrate the chemical origin of SEI formation by electrolyte reduction on lithium silicide thin films, synthesized by diffusion of pure evaporated lithium into smooth sputtered silicon. These model samples allowed for accurate estimation of irreversible capacity loss due to electrolyte reduction and for precise characterization of the resulting SEI by vibrational and photoelectron spectroscopies. Spectroscopic characterizations showed clear evidence that lithium silicide reduced electrolyte directly upon contact. Negligible first-cycle irreversible capacity loss was observed for the lithium silicide compared to silicon, indicating that the decomposition product of electrolyte on lithium silicide is able to stop further electrolyte reduction to a large extent. Fluoro-ethylene carbonate was shown to significantly affect the chemistry of electrolyte reduction on lithium silicide and subsequent cycling performance. The results of this basic study reveal the chemistry occurring at the interface of the lithium silicide and electrolyte and help in understanding the limitedmore »
- Authors:
-
- National Renewable Energy Lab. (NREL), Golden, CO (United States)
- Univ. of Colorado, Boulder, CO (United States)
- Publication Date:
- Research Org.:
- National Renewable Energy Lab. (NREL), Golden, CO (United States)
- Sponsoring Org.:
- USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V), Hybrid Electric Systems Program
- OSTI Identifier:
- 1515396
- Report Number(s):
- NREL/JA-5K00-72508
Journal ID: ISSN 1932-7447
- Grant/Contract Number:
- AC36-08GO28308
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Physical Chemistry. C
- Additional Journal Information:
- Journal Volume: 123; Journal Issue: 21; Journal ID: ISSN 1932-7447
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE; silicon anodes; lithium-ion batteries; energy storage; solid-electrolyte interphase formatioin
Citation Formats
Xu, Yun, Bloom, Aaron P., Coyle, Jaclyn E, Engtrakul, Chaiwat, Teeter, Glenn R., Stoldt, Conrad, Burrell, Anthony, and Zakutayev, Andriy A. Chemistry of Electrolyte Reduction on Lithium Silicide. United States: N. p., 2019.
Web. doi:10.1021/acs.jpcc.9b02611.
Xu, Yun, Bloom, Aaron P., Coyle, Jaclyn E, Engtrakul, Chaiwat, Teeter, Glenn R., Stoldt, Conrad, Burrell, Anthony, & Zakutayev, Andriy A. Chemistry of Electrolyte Reduction on Lithium Silicide. United States. https://doi.org/10.1021/acs.jpcc.9b02611
Xu, Yun, Bloom, Aaron P., Coyle, Jaclyn E, Engtrakul, Chaiwat, Teeter, Glenn R., Stoldt, Conrad, Burrell, Anthony, and Zakutayev, Andriy A. Tue .
"Chemistry of Electrolyte Reduction on Lithium Silicide". United States. https://doi.org/10.1021/acs.jpcc.9b02611. https://www.osti.gov/servlets/purl/1515396.
@article{osti_1515396,
title = {Chemistry of Electrolyte Reduction on Lithium Silicide},
author = {Xu, Yun and Bloom, Aaron P. and Coyle, Jaclyn E and Engtrakul, Chaiwat and Teeter, Glenn R. and Stoldt, Conrad and Burrell, Anthony and Zakutayev, Andriy A.},
abstractNote = {Silicon anodes are promising for next-generation lithium-ion batteries due to high theoretical capacity. However, their performance and lifetime are currently limited by continuous electrolyte reduction and solid-electrolyte interphase (SEI) formation. Thus, SEI studies are important but often complicated due to the rough morphology of samples, buried interfaces, and the presence of binders. Here, we demonstrate the chemical origin of SEI formation by electrolyte reduction on lithium silicide thin films, synthesized by diffusion of pure evaporated lithium into smooth sputtered silicon. These model samples allowed for accurate estimation of irreversible capacity loss due to electrolyte reduction and for precise characterization of the resulting SEI by vibrational and photoelectron spectroscopies. Spectroscopic characterizations showed clear evidence that lithium silicide reduced electrolyte directly upon contact. Negligible first-cycle irreversible capacity loss was observed for the lithium silicide compared to silicon, indicating that the decomposition product of electrolyte on lithium silicide is able to stop further electrolyte reduction to a large extent. Fluoro-ethylene carbonate was shown to significantly affect the chemistry of electrolyte reduction on lithium silicide and subsequent cycling performance. The results of this basic study reveal the chemistry occurring at the interface of the lithium silicide and electrolyte and help in understanding the limited calendar lifetime of Li-ion batteries with Si anodes.},
doi = {10.1021/acs.jpcc.9b02611},
journal = {Journal of Physical Chemistry. C},
number = 21,
volume = 123,
place = {United States},
year = {Tue May 07 00:00:00 EDT 2019},
month = {Tue May 07 00:00:00 EDT 2019}
}
Web of Science