Regulating Dynamic Dielectricity of Single-Ion Polymer Electrolytes via Polymerizable Deep Eutectic Monomer for Li thium Metal Batteries
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Deep eutectic solvents (DESs) have gained interest as potential replacements for conventional liquid electrolytes due to their non-flammability, low vapor pressure, and environmental friendliness. However, the free solvent in DESs has a low electrochemical stability window (ESW) below 4.0 V, and reactivity with lithium metal. Herein, we present a polymerizable deep eutectic monomer (PDEM)-based single-ion gel polymer electrolyte (SIGPE) to enhance ion transport and electrochemical stability. Ion-dipole bridges formed by PDEM create a dynamic nanophase with a high dielectric constant and superior viscoelasticity. This unique phenomenon suppresses Maxwell-Wagner-Sillars interfacial polarization from ions trapped in crystallized DES, enabling rapid ion transport through low binding energy of the solvation structure. The SIGPE shows a high ESW of 5.0 V and excellent performance in both Li symmetric and LFP cells, offering a novel strategy for high-performance lithium metal batteries.