Multiple Dynamic Bonds‐Driven Integrated Cathode/Polymer Electrolyte for Stable All‐Solid‐State Lithium Metal Batteries

Abstract

All‐solid‐state lithium metal batteries (LMBs) are considered as the promising higher‐energy and improved‐safety energy‐storage systems. Nevertheless, the electrolyte‐electrodes interfacial issues due to the limited solid physical contact lead to discontinuous interfacial charge transport and large interfacial resistance, thereby suffering from unsatisfactory electrochemical performance. Herein, we construct an integrated cathode/polymer electrolyte for all‐solid‐state LMBs under the action of polymer chains exchange and recombination originating from multiple dynamic bonds in our well‐designed dynamic supramolecular ionic conductive elastomers (DSICE) molecular structure. The DSICE acts as polymer electrolytes with excellent electrochemical performance and mechanical properties, achieving the ultrathin pure polymer electrolyte thickness (12 μm). Notably, the DSICE also functions as lithium iron phosphate (LiFePO4, LFP) cathode binders with enhanced adhesive capability. Such well‐constructed Li|DSICE|LFP‐DSICE cells generate delicate electrolyte‐electrodes interfacial contact at the molecular level, providing continuous Li+ transport pathways and promoting uniform Li+ deposition, further delivering superior long‐term charge/discharge stability (>600 cycles, Coulombic efficiency, >99.8 %) and high capacity retention (80 % after 400 cycles). More practically, the Li|DSICE|LFP‐DSICE pouch cells show stable electrochemical performance, excellent flexibility and safety under abusive tests.

Computational approach inspired advancements of solid-state electrolytes for lithium secondary batteries: from first-principles to machine learning

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In situ polymerization of solid-state polymer electrolytes for lithium metal batteries: a review

“…However, by far the most utilized is the induction of polymerization reactions by heat or UV light. In addition to free radical-initiated in situ polymerization, ionic polymerization, 84–86 polycondensation reactions 87,88 and electropolymerization 89,90 have also attracted much attention.…”

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