Ternary Hybrid Electrolyte with Regulating Zn-ion Flux for Highly Stable Flexible Na3V2(PO4)3-Zn Metal Quasi-Solid Battery

Achieving uniform ion flux both at the interface and in the matrix simultaneously remains a challenge with current liquid/solid electrolytes. Herein, we demonstrate a novel strategy to address the issue by designing and synthesizing a polyvinylidene fluoride hexafluoropropylene (PVDF-HFP) based ternary hybrid electrolyte (PTHE). In this unique material architecture, each component synergistically serves a specific purpose: The PVDF-HFP-Zn(OTF) 2 serves as the stable electrolyte skeleton, providing the ion transport network. The Cu-MOF regulates the Zn 2+ solvation structure and anion distribution, achieving uniform ion flux in the electrolyte matrix. Moreover, the thin liquid electrolyte film at the interface promotes ion transport and stabilizes the electrode-electrolyte interface. The PTHE exhibits balanced high performance with respect to cycling stability (3200 h at 0.2 mA cm −2 ) and excellent capacity retention when paired with the Na 3 V 2 (PO 4 ) 3 (NVP) cathode (0.0029 % capacity decay per cycle after 2000 cycles at 0.5 A g −1 ), alongside uniform Zn metal deposition and effective dendrite suppression. Furthermore, the PTHE based NVP-Zn metal quasi-solid battery demonstrates outstanding flexibility (enduring 1000 bending cycles with less than 10% decrease in capacity retention), owing to the existence of the thin liquid electrolyte film. This work provides a novel strategy for developing highly stable flexible NVP-Zn metal quasi-solid batteries by synergistically optimizing ion flux both at the interface and in the matrix.