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Interfacial thermal transport between electrodes and polymer electrolytes canplay a crucial role in the thermal management of solid-state lithium-ionbatteries (SLIBs). Modifying the electrode surface with functional moleculescan effectively increase the interfacial thermal conductance (ITC) betweenelectrodes and polymers (e.g., electrolytes, separators); however, how theyinfluence the interfacial thermal transport in SLIBs during charge/dischargeremains unknown. In this work, we conduct molecular dynamics (MD) simulationsto investigate the ITC between charged electrodes and solid-state polymerelectrolytes (SPEs) mixed with ionic liquids (ILs). We find that ILs could selfassemble at the electrode surface and act as non-covalent functional moleculesthat could significantly enhance the interfacial thermal transport duringcharge/discharge because of the formation of a densely packed cationic oranionic layer at the interface. While the electrostatic interactions betweenthe charged electrode and the IL ions are responsible for forming these denseinterfacial layers, the enhancement of ITC is mainly contributed by theincreased Lennard-Jones (LJ) interactions between the charged electrodes andILs. This work may provide useful insights into the understanding ofinterfacial thermal transport between electrodes and electrolytes of SLIBsduring charge/discharge.

Enhanced Thermal Transport across the Interface between Charged Graphene  Electrodes and Poly(ethylene oxide) Electrolytes by Non-covalent  Functionalization