Silicon Surface Tethered Polymer as Artificial Solid Electrolyte Interface
Abstract
Here, we have developed a proof of concept electrode design to covalently graft poly(methyl methacrylate) brushes directly to silicon thin film electrodes via surface-initiated atom transfer radical polymerization. This polymer layer acts as a stable artificial solid electrolyte interface that enables surface passivation despite large volume changes during cycling. Thin polymer layers (75 nm) improve average first cycle coulombic efficiency from 62.4% in bare silicon electrodes to 76.3%. Average first cycle reversible capacity was improved from 3157 to 3935 mAh g-1, and average irreversible capacity was reduced from 2011 to 1020 mAh g-1. Electrochemical impedance spectroscopy performed on silicon electrodes showed that resistance from solid electrolyte interface formation increased from 79 to 1508 Ω in untreated silicon thin films over 26 cycles, while resistance growth was lower – from 98 to 498 Ω – in silicon films functionalized with PMMA brushes. The lower increase suggests enhanced surface passivation and lower electrolyte degradation. This work provides a pathway to develop artificial solid electrolyte interfaces synthesized under controlled reaction conditions.
- Authors:
-
[2];
- Univ. of Rochester, NY (United States). Dept. of Chemical Engineering
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division
- Publication Date:
- Research Org.:
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1462871
- Grant/Contract Number:
- AC05-00OR22725
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Scientific Reports
- Additional Journal Information:
- Journal Volume: 8; Journal ID: ISSN 2045-2322
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE
Citation Formats
Shen, Brian H., Veith, Gabriel M., and Tenhaeff, Wyatt E. Silicon Surface Tethered Polymer as Artificial Solid Electrolyte Interface. United States: N. p., 2018.
Web. doi:10.1038/s41598-018-30000-z.
Shen, Brian H., Veith, Gabriel M., & Tenhaeff, Wyatt E. Silicon Surface Tethered Polymer as Artificial Solid Electrolyte Interface. United States. https://doi.org/10.1038/s41598-018-30000-z
Shen, Brian H., Veith, Gabriel M., and Tenhaeff, Wyatt E. Wed .
"Silicon Surface Tethered Polymer as Artificial Solid Electrolyte Interface". United States. https://doi.org/10.1038/s41598-018-30000-z. https://www.osti.gov/servlets/purl/1462871.
@article{osti_1462871,
title = {Silicon Surface Tethered Polymer as Artificial Solid Electrolyte Interface},
author = {Shen, Brian H. and Veith, Gabriel M. and Tenhaeff, Wyatt E.},
abstractNote = {Here, we have developed a proof of concept electrode design to covalently graft poly(methyl methacrylate) brushes directly to silicon thin film electrodes via surface-initiated atom transfer radical polymerization. This polymer layer acts as a stable artificial solid electrolyte interface that enables surface passivation despite large volume changes during cycling. Thin polymer layers (75 nm) improve average first cycle coulombic efficiency from 62.4% in bare silicon electrodes to 76.3%. Average first cycle reversible capacity was improved from 3157 to 3935 mAh g-1, and average irreversible capacity was reduced from 2011 to 1020 mAh g-1. Electrochemical impedance spectroscopy performed on silicon electrodes showed that resistance from solid electrolyte interface formation increased from 79 to 1508 Ω in untreated silicon thin films over 26 cycles, while resistance growth was lower – from 98 to 498 Ω – in silicon films functionalized with PMMA brushes. The lower increase suggests enhanced surface passivation and lower electrolyte degradation. This work provides a pathway to develop artificial solid electrolyte interfaces synthesized under controlled reaction conditions.},
doi = {10.1038/s41598-018-30000-z},
journal = {Scientific Reports},
number = ,
volume = 8,
place = {United States},
year = {Wed Aug 01 00:00:00 EDT 2018},
month = {Wed Aug 01 00:00:00 EDT 2018}
}
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Application of A-C Techniques to the Study of Lithium Diffusion in Tungsten Trioxide Thin Films
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Silicon/Graphite Composite Electrodes for High-Capacity Anodes: Influence of Binder Chemistry on Cycling Stability
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- Electrochemical and Solid-State Letters, Vol. 11, Issue 5
Silane-Derived SEI Stabilization on Thin-Film Electrodes of Nanocrystalline Si for Lithium Batteries
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The Mechanism of SEI Formation on a Single Crystal Si(100) Electrode
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Analysis of Three-Electrode Setups for AC-Impedance Measurements on Lithium-Ion Cells by FEM simulations
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