Charge Transfer in Ultrafine LDH Nanosheets/Graphene Interface with Superior Capacitive Energy Storage Performance

Two-dimensional LDH nanosheets recently have generated considerable interest in various promising applications because of their intriguing properties. Herein, we report a facile in situ nucleation strategy toward in situ decorating monodispersed Ni-Fe LDH ultrafine nanosheets (UNs) on graphene oxide template based on the precise control and manipulation of LDH UNs anchored, nucleated, grown, and crystallized. Anion-exchange behavior was observed in this Ni-Fe LDH UNs@rGO composite. The Ni-Fe LDH UNs@rGO electrodes displayed a significantly enhanced specific capacitance (2715F g^-1 at 3 A g^-1) and energy density (82.3 Wh kg^-1 at 661 W kg^-1), which exceeds the energy densities of most previously reported nickel iron oxide/hydroxides. Moreover, the asymmetric supercapacitor, with the Ni-Fe LDH UNs @rGO composite as the positive electrode material and reduced graphene oxide (rGO) as the negative electrode material, exhibited a high energy density (120 Wh kg ^-1) at an average power density of 1.3 kW kg ^-1. A charge transfer from LDH layer to graphene layer, which means a built in electric field directed from LDH to graphene can be established by DFT calculations, which can significantly accelerate reaction kinetics and effectively optimize the capacitive energy storage performance.