Simultaneous Structure, Thermal, and Mechanics Regulation for Boosting Performance of PVDF-Based Solid-State Electrolytes.

Poly(vinylidene fluoride) (PVDF) is promising for polymer solid-state electrolytes (PSEs) but faces challenges such as low ionic conductivity, uneven strain distribution, and poor lithium (Li) dendrite inhibition. Herein, an effective strategy is proposed to enhance PVDF-based PSEs by incorporating a fast ion conductor LiZr(PO) (LZP) with a negative thermal expansion property and a NASICON-type structure, and the effects are investigated using multifarious methods. The added LZP not only enhances the mobility of the PVDF chain and the concentration of free Li, but regulates heat release and volume expansion of PSEs during cycles, thereby protecting electrode morphology and structure, as well as improving the interface between the electrode and electrolyte.