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Composite polymer electrolytes (CPEs) incorporate the advantages of solid polymer electrolytes (SPEs) and inorganic solid electrolytes (ISEs), which have shown huge potential in the application of safe lithium-metal batteries (LMBs). Effectively avoiding the agglomeration of inorganic fillers in the polymer matrix during the organic–inorganic mixing process is very important for the properties of the composite electrolyte. Herein, a partial cross-linked PEO-based CPE was prepared by porous vinyl-functionalized silicon (p-V-SiO 2 ) nanoparticles as fillers and poly (ethylene glycol diacrylate) (PEGDA) as cross-linkers. By combining the mechanical rigidity of ceramic fillers and the flexibility of PEO, the as-made electrolyte membranes had excellent mechanical properties. The big special surface area and pore volume of nanoparticles inhibited PEO recrystallization and promoted the dissolution of lithium salt. Chemical bonding improved the interfacial compatibility between organic and inorganic materials and facilitated the homogenization of lithium-ion flow. As a result, the symmetric Li|CPE|Li cells could operate stably over 450 h without a short circuit. All solid Li|LiFePO 4  batteries were constructed with this composite electrolyte and showed excellent rate and cycling performances. The first discharge-specific capacity of the assembled battery was 155.1 mA h g −1 , and the capacity retention was 91% after operating for 300 cycles at 0.5 C. These results demonstrated that the chemical grafting of porous inorganic materials and cross-linking polymerization can greatly improve the properties of CPEs.

Excellent Performances of Composite Polymer Electrolytes with Porous Vinyl-Functionalized SiO2 Nanoparticles for Lithium Metal Batteries