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Swapping Conventional Salts with Entrapped Lithiated Anionic Polymer: Fast Single-Ion Conduction and Electrolyte Feasibility in LiFePO4/Li Batteries

Abstract

Herein, we report on a new class of quasi-solid polymer electrolyte matrix that supports appreciably fast single-ion conduction. Showcased as the first example of tailoring a lithiated anionic polymer employing a semi-interpenetrating polymer networks approach, the study probes several key factors, such as, (i)polymer-polymer/ion-polymer interactions (ii) phase homogeneity, (iii) effect of oligomeric plasticization, (iv) transition temperatures and thermostability, (v) H-bonding and degree of crystallinity for a series of binary and ternary compositions, and determines their role on the overall electrochemical properties. Employing a mutually exclusive reaction strategy, lithiated poly(3-sulfopropyl methacrylate) was synthesized via free-radical polymerization and interpenetrated into a growing polyether-polyurethane networks to achieve solid free standing films. Quantitative cation exchange, polymerization and network incorporation are confirmed by 1H-, 13C-NMR, XRD, ICP-OES, ESI-MS, MALDI-TOF and mid-FTIR. Comprehensive evaluations of physico-chemical and electrochemical properties provide crucial understanding on the microscopic contributions of the coexisting phases and correlated charge transport behavior. Unlike the Grotthuss mechanism foreseen for single-ion conduction, interestingly, the findings strongly indicates that the charge transport is preferentially promoted within the ether cages that acts as ion-channels. Impressively, ionic conductivity, σ ≅ 10-5-10-4 Scm-1 with an estimated cationic transport number, tLi+ > 0.87 at ambient temperatures and electrochemical stability > 4.7 V could be achieved with composition optimization, which is almost an order more than the documented reports on single-ion conductors. A feasibility study in a LiFePO4/SIC-PE/Li system underscores their potential viability with encouraging preliminary results.

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Supplementary files

Publication details

The article was received on 15 Feb 2017, accepted on 19 May 2017 and first published on 19 May 2017


Article type: Paper
DOI: 10.1039/C7TA01431G
Citation: J. Mater. Chem. A, 2017, Accepted Manuscript
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    Swapping Conventional Salts with Entrapped Lithiated Anionic Polymer: Fast Single-Ion Conduction and Electrolyte Feasibility in LiFePO4/Li Batteries

    S. Gowneni and P. Basak, J. Mater. Chem. A, 2017, Accepted Manuscript , DOI: 10.1039/C7TA01431G

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