skip to main content

DOE PAGESDOE PAGES

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