November 30, 2025Nano Letters0 citations

Covalent Organic Framework Mediated Solvation in Quasi-Solid-State Polymer Electrolyte for High-Performance Silicon-Based Lithium-Ion Batteries

Key Points

Ionic conductivity of the COF-based quasi-solid-state polymer electrolyte reached 2.99 mS cm-1, enabling better battery performance.
After 500 cycles, Si anodes delivered a specific capacity of 1722 mAh g-1, demonstrating high performance.
Analysis of the role of lithiated covalent organic frameworks in enhancing ionic migration and desolvation was conducted with advanced techniques.
Findings suggest that COF-modulated designs may lead to improvements in the stability of solid-state lithium-ion batteries.

Abstract

The practical application of solid polymer electrolytes (SPEs) is limited by their low ionic conductivity and poor interfacial compatibility with silicon (Si) anodes in high-energy-density, safe lithium-ion batteries (LIBs). Here, we introduce a lithiated covalent organic framework (COF) into a poly(vinylidene fluoride-cohexafluoropropylene) (PVDF-HFP)-based quasi-solid polymer electrolyte (QSPE) containing plasticizers to increase its electrochemical performance. The resulting COF-based QSPE has a high ionic conductivity of 2.99 mS cm-1 and enables Si anodes to deliver a remarkable specific capacity of 1722 mAh g-1 after 500 cycles, along with an excellent rate capability of up to 10 A g-1. Furthermore, we provide new insights into the role of lithiated COFs in modulating the Li+ solvation structure, facilitating ionic migration and promoting desolvation in plasticizer-containing solid electrolytes at the molecular scale. These findings offer valuable guidelines for the rational design of stable Si anodes in solid-state batteries.

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