Novel configuration of poly(vinylidenedifluoride)-based gel polymer electrolyte for application in lithium-ion batteries

Herein we propose a novel poly(vinylidene difluoride) (PVdF)-based gel polymer electrolyte (GPE) for application in lithium-ion batteries, LIBs. The GPE is prepared under air as a dry, flexible film and directly gelled during LIB assembly with a conventional liquid organic electrolyte. The dry-gel here originally reported maintains its structural integrity due to the presence of crystallized EC-solvent within its matrix that avoids structural collapse, as demonstrated by TGA analysis. By avoiding the use of controlled atmosphere, the GPE is easy to handle and suitable for roll-to-roll scaling-up, i.e. characteristics missed by the common gel membranes. Scanning Electron Microscopy (SEM) evidences a micrometric polymer network of the dry membrane precursor acting as the support matrix for the gelation. Electrochemical impedance spectroscopy (EIS) measurements and galvanostatic tests suggest a good stability of the lithium electrode/gel electrolyte interface and a satisfactory lithium transference number. Cycling tests of gel-electrolyte-based lithium half-cells using lithium iron phosphate (LiFePO4, LFP) and graphite (C), respectively, as counter electrodes, as well as of a full C/LFP lithium-ion battery confirm the suitability of the GPE developed in this work for application in stable, low cost and environmentally friendly energy storage systems.