High-Entropy Microdomain Interlocking Polymer Electrolytes for Advanced All-Solid-State Battery Chemistries.
basic_science · Level V
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- Record sourced from PubMed, PMID 36341499.
- Also identified by DOI 10.1002/adma.202209402.
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Abstract
All-solid-state polymer electrolytes (ASPEs) with excellent processivity are considered one of the most forward-looking materials for large-scale industrialization. However, the contradiction between improving the mechanical strength and accelerating the ionic migration of ASPEs has always been difficult to reconcile. Herein, a rational concept is raised of high-entropy microdomain interlocking ASPEs (HEMI-ASPEs), inspired by entropic elasticity well-known in polymer and biochemical sciences, by introducing newly designed multifunctional ABC miktoarm star terpolymers into polyethylene oxide for the first time. The tailor-made HEMI-ASPEs possess multifunctional polymer chains, which induce themselves to assemble into micro- and nanoscale dynamic interlocking networks with high topological structure entropy. HEMI-ASPEs achieve excellent toughness, considerable ionic conductivity, an appreciable lithium transference number (0.63), and desirable thermal stability (T<sub>d</sub> > 400 °C) for all-solid-state lithium metal batteries. The Li|HEMI-ASPE-Li|Li symmetrical cell shows a stable Li plating/stripping performance over 4000 h, and a LiFePO<sub>4</sub> |HEMI-ASPE-Li|Li full cell exhibits a high capacity retention (≈96%) after 300 cycles. This work contributes an innovative design concept introducing high-entropy supramolecular dynamic networks for ASPEs.