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Title: Silicon Surface Tethered Polymer as Artificial Solid Electrolyte Interface

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:
 [1] ; ORCiD logo [2] ;  [1]
  1. Univ. of Rochester, NY (United States). Dept. of Chemical Engineering
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division
Publication Date:
Grant/Contract Number:
AC05-00OR22725
Type:
Accepted Manuscript
Journal Name:
Scientific Reports
Additional Journal Information:
Journal Volume: 8; Journal ID: ISSN 2045-2322
Publisher:
Nature Publishing Group
Research Org:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE
OSTI Identifier:
1462871

Shen, Brian H., Veith, Gabriel M., and Tenhaeff, Wyatt E.. Silicon Surface Tethered Polymer as Artificial Solid Electrolyte Interface. United States: N. p., 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. doi:10.1038/s41598-018-30000-z.
Shen, Brian H., Veith, Gabriel M., and Tenhaeff, Wyatt E.. 2018. "Silicon Surface Tethered Polymer as Artificial Solid Electrolyte Interface". United States. doi: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 = {2018},
month = {8}
}

Works referenced in this record:

A review of polymer dissolution
journal, August 2003

A review of the features and analyses of the solid electrolyte interphase in Li-ion batteries
journal, September 2010

Atom Transfer Radical Polymerization (ATRP): Current Status and Future Perspectives
journal, April 2012
  • Matyjaszewski, Krzysztof
  • Macromolecules, Vol. 45, Issue 10, p. 4015-4039
  • DOI: 10.1021/ma3001719