Solvent-Induced Complexation-to-Disentanglement Strategy for the Selective and Green Recovery of Nanoplastic PVDF Polymer Solid Electrolytes in Spent All-Solid-State Batteries

The large-scale commercialization of all-solid-state batteries (ASSBs) is expected to generate substantial quantities of spent polyvinylidene fluoride (PVDF)-based polymer solid electrolytes (PSEs) in the near future. The accumulation of these spent PVDF nanoplastic poses significant risks of environmental pollution and resource waste, underscoring the urgent need for efficient and environmentally friendly methods for PVDF recycling. Here, we propose, for the first time, a solvent-induced complexation-to-disentanglement (SICD) strategy for the selective recovery of nanoscale PVDF-based PSEs from spent ASSBs. Remarkably, the SICD approach enables green and efficient PVDF recycling, achieving a fluorine leaching efficiency that is approximately 75 times higher than that of lithium in metal-contained solid-state electrolytes at a mild temperature within 2 h. Such high selectivity is primarily attributed to the initial complexation of PVDF by green solvents, followed by the cleavage of C–F bonds leading to polymer disentanglement.