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Tailoring electrolyte coordination structure for high-rate polymer-based solid-state batteries
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DOI：10.1039/D5SC07849K.png)
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Abstract
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Solid-state batteries (SSBs) offer intrinsic safety and superior energy density; promising next-generation energy storage. Polymer-based solid-state electrolytes (SSEs) stand out for their facile processing and low cost. However; the development of SSBs is impeded by the intrinsically low ionic conductivity of polymer electrolytes at room temperature; alongside limitations in their inherent electrochemical stability and thermal resilience. Here; we propose a novel solvation-tailoring strategy by embedding 3D continuously interconnected zirconium-based metal–organic framework (MOF808) nanofillers into a polyvinylidene fluoride–hexafluoropropylene (PVDF–HFP) matrix (designated as PLM-3). This design leverages the strong adsorption of MOF808 for solvent molecules (−0.521 eV) to thermodynamically displace them from the Li+ solvation sheath; replacing them with anions and forming an anion-enriched coordination configuration. This precisely tailored solvation environment; quantified by a surge in anion-aggregate (AGG) species; significantly enhances Li+ transport kinetics by reducing Li+ desolvation energy by 15.8% (−5.29 vs. −6.28 eV); thereby endowing the resultant electrolyte with exceptional rate performance. When coupled with a high voltage single-crystal NCM83 (SC-NCM83) cathode; the PLM-3 cell delivers exceptional rate capability (219.5 mAh g−1 at 0.1C; 182.8 mAh g−1 at 5C) while maintaining 93.73% capacity retention after 200 cycles at 1C with a 4.3 V cutoff voltage. This solvation-tailoring strategy thus redefines the rate limits of polymer-based SSBs and paves the way for the development of high-power; high-energy; and industrially viable SSBs.
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