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Solid-state polymer electrolytes hold significant promise as a cornerstone technology for developing high-energy-density lithium metal batteries, thanks to their cost-effectiveness, superior safety, and exceptional interfacial compatibility. Nevertheless, their widespread industrial adoption has been hindered by challenges such as relatively low ionic conductivity and lithium-ion transference numbers. Enhancing the performance of solid-state batteries has long hinged on the ability to decouple lithium-ion transport from the segmental motion of polymer chains. To date, research efforts have predominantly centered on material structure design and performance enhancement, yet a comprehensive understanding of the atomic-level dynamic mechanisms governing ion transport and their intricate structure-activity relationships remains elusive.
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