The development of chemically stable and high conductive membranes is one of the most important issues to improve the performance of vanadium flow batteries (VFBs). Herein, poly(vinylidene fluoride) (PVDF)/graphene composite nanoporous membranes were easily fabricated by manipulating crystallization processes. The graphene was used to enhance membrane selectivity and conductivity. In the nanoscale channels of the membranes, the graphene nanosheets reduced the apertures among the crystal grains, thus restraining vanadium ions crossover due to the size exclusion effect. Moreover, the oxygen groups on the graphene improved the surface hydrophilicity and formed hydrogen bonds with the PVDF polymer chains, which facilitated the proton transport. The composite membranes, with a 0.15 wt % graphene loading, showed a selectivity of 38.2 and conductivity of 37.1 mS/cm. The single cell exhibited a coulomb efficiency of 94.7%, a voltage efficiency of 88.5%, and an energy efficiency of 83.8%, which was 13% higher than that of the pristine PVDF membranes. The composite membranes showed excellent stability during 100 charge-discharge cycles. All these results indicate that the PVDF/graphene composite membrane is a promising candidate for VFB applications.
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