ARGET-ATRP-Mediated Grafting of Bifunctional Polymers onto Silica Nanoparticles Fillers for Boosting the Performance of High-Capacity All-Solid-State Lithium–Sulfur Batteries with Polymer Solid Electrolytes

The shuttle effect in lithium–sulfur batteries, which leads to rapid capacity decay, can be effectively suppressed by solid polymer electrolytes. However, the lithium-ion conductivity of polyethylene oxide-based solid electrolytes is relatively low, resulting in low reversible capacity and poor cycling stability of the batteries. In this study, we employed the activator generated through electron transfer atom transfer radical polymerization to graft modify the surface of silica nanoparticles with a bifunctional monomer, 2-acrylamide-2-methylpropanesulfonate, which possesses sulfonic acid groups with low dissociation energy for facilitating Li+ migration and transfer, as well as amide groups capable of forming hydrogen bonds with polyethylene oxide chains. Subsequently, the modified nanoparticles were blended with polyethylene oxide to prepare a solid polymer electrolyte with low crystallinity and high ion conductivity. The resulting electrolyte demonstrated excellent and stable electrochemical performance, with a discharge-specific capacity maintained at 875.2 mAh g−1 after 200 cycles.