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Title: Decoupling the Ionic Conductivity and Elastic Modulus of Gel Electrolytes: Fully Zwitterionic Copolymer Scaffolds in Lithium Salt/Ionic Liquid Solutions
Abstract

A critical barrier to overcome in the development of solid‐state electrolytes for lithium batteries is the trade‐off between sacrificing ionic conductivity for enhancement of mechanical stiffness. Here, a physically cross‐linked, polymer‐supported gel electrolyte consisting of a lithium salt/ionic liquid solution featuring a fully zwitterionic (ZI) copolymer network is introduced for rechargeable lithium‐based batteries. The ZI scaffold is synthesized using a 3:1 molar ratio of 2‐methacryloyloxyethyl phosphorylcholine and sulfobetaine vinylimidazole, and the total polymer content is varied between 1.1 and 12.5 wt%. Room‐temperature ionic conductivity values comparable to the base liquid electrolyte (≈1 mS cm−1) are achieved in ZI copolymer‐supported gels that display compressive elastic moduli as large as 14.3 MPa due to ZI dipole–dipole cross‐links. Spectroscopic characterization suggests a change in the Li+coordination shell upon addition of the zwitterions, indicative of strong Li+···ZI group interactions. Li+transference number measurements reveal an increase in Li+conductivity within a ZI gel electrolyte (nearly doubles). ZI gels display enhanced stability against Li metal, dendrite suppression, and suitable charge–discharge performance in a graphite|lithium nickel cobalt manganese oxide cell. Fully ZI polymer networks in nonvolatile, ionic liquid‐based electrolytes represent a promising approach toward realizing highly conductive, mechanically rigid gels for lithium battery technologies.

 
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PAR ID:
10066091
Author(s) / Creator(s):
 ;  
Publisher / Repository:
Wiley Blackwell (John Wiley & Sons)
Date Published:
Journal Name:
Advanced Energy Materials
Volume:
8
Issue:
26
ISSN:
1614-6832
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
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