Silicon Surface Tethered Polymer as Artificial Solid Electrolyte Interface

Brian H. Shen, Gabriel M. Veith, Wyatt E. Tenhaeff

Research output: Contribution to journalArticlepeer-review

24 Scopus citations

Abstract

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.

Original languageEnglish
Article number11549
JournalScientific Reports
Volume8
Issue number1
DOIs
StatePublished - Dec 1 2018

Bibliographical note

Publisher Copyright:
© 2018, The Author(s).

Funding

This material is based upon work supported by the U.S. Department of Energy, Office of Science, Office of Workforce Development for Teachers and Scientists, Office of Science Graduate Student Research (SCGSR) program (BHS). The SCGSR program is administered by the Oak Ridge Institute for Science and Education for the DOE under contract number DE-SC0014664. This work was supported by the National Science Foundation under IGERT award #DGE-0966089 (BHS). The synthesis work was supported by the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Materials Science and Engineering (GMV).

FundersFunder number
Division of Materials Science and Engineering
GMV
Office of Basic Energy Sciences
Office of Science Graduate Student Research
SCGSR
National Science Foundation
U.S. Department of EnergyDE-SC0014664
Directorate for Education and Human Resources0966089
Office of Science
Workforce Development for Teachers and Scientists
Oak Ridge Institute for Science and Education

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