Supramolecular polymer cross-linking gel electrolyte for highly stable quasi-solid-state lithium metal batteries

Lithium (Li) metal batteries have the advantage of high energy density, but the Li dendrites risk piercing the separator and causing a short circuit in the battery. Replacing the liquid electrolytes with gel electrolytes is considered an effective strategy to solve the issues. Herein, a poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP)-based gel electrolyte, improved with multifunctional supramolecular polymer (MSP), was prepared to enhance the cycling stability and energy density of quasi-solid-state Li metal batteries. The MSP addictive constructs a cross-linked network structure with PVDF-HFP matrix and lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) through hydrogen bonding, improving the mechanical strength of the composite gel electrolyte (PH-10%MSP-GE) to against the growth of Li dendrites. Moreover, the pre-lithiated sulfonic acid groups, conductive polyether groups of MSP, and the attraction of TFSI^- anions, promote the Li-ion transportation of the composite gel electrolyte. Finally, the Li||Li symmetric cell cycle stably for over 450 h. The Li||LiFePO₄ full cell demonstrates a high energy density and excellent cycling stability for over 600 cycles, with a capacity retention rate of up to 98.7%. This work provides valuable insights into the preparation of multifunctional composite gel polymer electrolytes and competitive quasi-solid-state Li metal batteries.