Affiliation:
1. Department of Chemical & Biomolecular Engineering University of Maryland 4418 Stadium Dr College Park MD 20740 USA
2. Department of Physics & Astronomy Hunter College of the City University of New York 695 Park Ave New York NY 10065 USA
3. Department of Materials Science & Engineering University of Maryland 4418 Stadium Dr College Park MD 20740 USA
4. Battery Science Branch, Energy Science Division, Sensors and Electron Devices Directorate DEVCOM US Army Research Laboratory 2800 Powder Mill Rd Adelphi MD 20783 USA
Abstract
AbstractSolid polymer electrolytes (SPEs) have the potential to meet evolving Li‐ion battery demands, but for these electrolytes to satisfy growing power and energy density requirements, both transport properties and electrochemical stability must be improved. Unfortunately, improvement in one of these properties often comes at the expense of the other. To this end, a “hybrid aqueous/ionic liquid” SPE (HAILSPE) which incorporates triethylsulfonium‐TFSI (S2,2,2) or N‐methyl‐N‐propylpyrrolidinium‐TFSI (Pyr1,3) ionic liquid (IL) alongside H2O and LiTFSI salt to simultaneously improve transport and electrochemical stability is studied. This work focuses on the impact of HAILSPE composition on electrochemical performance. Analysis shows that an increase in LiTFSI content results in decreased ionic mobility, while increasing IL and water content can offset its impact. pfg‐NMR results reveal that preferential lithium‐ion transport is present in HAILSPE systems. Higher IL concentrations are correlated with an increased degree of passivation against H2O reduction. Compared to the Pyr1,3 systems, the S2,2,2 systems exhibit a stronger degree of passivation due to the formation of a multicomponent interphase layer, including LiF, Li2CO3, Li2S, and Li3N. The results herein demonstrate the superior electrochemical stability of the S2,2,2 systems compared to Pyr1,3 and provide a path toward further enhancement of HAILSPE performance via composition optimization.
Funder
National Science Foundation
Army Research Laboratory
Subject
General Materials Science,Renewable Energy, Sustainability and the Environment
Cited by
2 articles.
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