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Title: Silicon Surface Tethered Polymer as Artificial Solid Electrolyte Interface

Journal Article · · Scientific Reports
 [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

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.

Research Organization:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC05-00OR22725
OSTI ID:
1462871
Journal Information:
Scientific Reports, Vol. 8; ISSN 2045-2322
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 22 works
Citation information provided by
Web of Science

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Cited By (2)

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