Polymer-mediated vacancy defects of graphene sheets as high-performance cathode materials for aqueous zinc-ion hybrid supercapacitors

The electrochemical behavior of graphene sheets in energy storage system is closely related to its electronic structures. Specifically, structural vacancy defects can expose more active sites and enhance the electrochemical performance. However, it is still a challenging problem to realize valid defect regulation on improving the reaction kinetics of electrode materials. Herein, vacancy-defective graphene sheets were constructed through the thermal mediated method via intercalation of polyacrylonitrile nanofibers. The vacancy defects were generated from the NH₃ gas resulting from polymer decomposition at gradient carbonization temperature. The obtained composites of the graphene sheets and carbon nanofibers demonstrate that the vacancy defects benefit to charge transport, allowing more electrons to pass through the interlayered structure, and enhance the adsorption capacitance during the reversible electrochemical process. In addition, the as-assembled Zn ion hybrid supercapacitors exhibit a high energy density of 129.9 Wh kg⁻¹ and outstanding cyclic stability (99.8 % after 10,000 cycling). The confined polymer-mediated thermal modification strategy can afford abundant vacancy defective sites and exhibit promising outlook for constructing high-performance graphene-based electrode materials for Zn ion hybrid supercapacitors.