Abstract

The present article entails development of an elastomeric, highly conductive, polymer electrolyte membrane (PEM) network via acrylate functionalization of poly(ethylene glycol) – block – poly(propylene glycol) – block – poly(ethylene glycol) (PEG-b-PPG-b-PEG) as a photocurable macromonomer and subsequent evaluation on electrochemical performance. By mixing as-synthesized macromonomer with ethylene carbonate (EC) plasticizer and lithium bis(trifluoromethane sulfonyl) imide (LiTFSI) salt, homogeneous melt mixtures were obtained over a wide range of compositions. Upon photopolymerization within the isotropic region, the UV-cured ternary mixture remained transparent and homogeneous, forming an elastomeric PEM network. The polymer electrolyte network-based PEM/EC/LiTFSI (20/40/40) exhibited a superionic conductivity level of ∼10−3 S/cm at room temperature; similarly other PEM compositions reached the superconductor level at battery operating temperatures of 40 ∼ 50 °C with improved thermal resistance and high elongation-at-break over 100%. The PEM further reveals a wide electrochemical window (-0.5 ∼ 4.5 V) with reasonably good capacity retention at ambient temperature of about 89%, and Coulombic efficiency of almost 100% after 50 cycles, determined by galvanostatic charge-discharge cycling at the C/3 rate.

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