A Solid Polymer Electrolyte from Photo-Crosslinked Polytetrahydrofuran and a Cycloaliphatic Epoxide for Lithium-Ion Cond

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MRS Advances © 2020 Materials Research Society DOI: 10.1557/adv.2020.274

A Solid Polymer Electrolyte from PhotoCrosslinked Polytetrahydrofuran and a Cycloaliphatic Epoxide for Lithium-Ion Conduction Francielli S. Genier,1 James Barna,2 Jiayue Wang,1 Saeid Biria, 1 Ian D. Hosein1* Syracuse University, Department of Biomedical and Chemical Engineering, Syracuse, NY, 13244

Cazenovia High School, Cazenovia, NY, 13035.

ABSTRACT

We report on the synthesis, properties, and ion conductivity of a solid polymer electrolyte produced from polytetrahydrofuran (PTHF) photo-crosslinked with 3,4epoxycyclohexylmethyl 3ʹ,4ʹ-epoxycyclohexane carboxylate (Epoxy), via an active monomer mechanism that facilitates the reaction of the native hydroxyl and epoxide endgroups. Crosslinked samples were loaded with different quantities of lithium tetrafluoroborate (LiBF4) and evaluated by electrochemical spectroscopy impedance (EIS) to determine their ionic conductivity. An increase in lithium salt loading led to an increase in ionic transport, reaching competitive conductivities of up to 10 -3 S/cm at temperatures typical for battery operation. Thermal analysis confirms the amorphous structure and high thermal stability (30-90°). The mechanical analysis shows the materials possess suitable stiffness for applications. The results demonstrate a new synthetic route to tunable crosslinked networks for a broad range of chemical building blocks to achieve high lithium-ion conduction and attain desirable thermal and mechanical properties.

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Keywords: solid polymer electrolyte, crosslinking, lithium conduction, polytetrahydrofuran. Corresponding Author: Ian D. Hosein (*[email protected], 315.443.4126)

INTRODUCTION The development of high-performance batteries is central to meeting global energy demands, while also storing energy in a clean, affordable, and safe manner. Towards this end, a research area of intense focus has been the replacement of the liquid or gel electrolyte with a solid polymer material, namely a solid polymer electrolyte (SPE). SPEs could enable batteries with higher energy density by allowing the use of lithium metal anode. They could also further address concerns over the volatility and flammability of currently used organic solvents.1–3 For a solid material to feasibly replace either a liquid or a gel electrolyte, it needs to have high conductivity and mechanical stability. That comes with an inherent trade-off: softer materials enable higher conductivity via more rapid chain relaxation to enable quick transport of the ions across the polymer chain, yet stiffer materials provide better mechanical integrity at the expense of conductivity. 4 Additionally, this trade-off must be considered with the space of constituents that maintain the thermal stability of the SPE in the battery temperature window. In t