Expanding hydrated vanadate with transition metal cations collectively promotes and catalyzes fast and more Zn-ion intercalation in aqueous batteries.

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Layered double hydroxides (LDHs) have attracted tremendous interest for applications in energy harvest and storage. However, the aggregation of nanosheets compromises the accessible active sites and limits their electrochemical performance, especially at high rates. The present study reports the synthesis of highly dispersed NiFe-LDH nanosheets anchored on reduced graphene oxide (NiFe-LDH/rGO) composites chemically bonded via a facile one-step hydrothermal method. Defect-riched rGO provides abundant active sites for heterogeneous nucleation of NiFe-LDH nanosheets, achieving the much efficient charge transfer between rGO and NiFe-LDH as compared to physically mixed NiFe-LDH + rGO. The crystallite size can effectively reduce to 5.5 nm smaller than 15.1 nm of NiFe-LDH without rGO, beneficial to expose more active surface for fast ion diffusion and redox reactions. NiFe-LDH/rGO as an anode material in lithium-ion batteries shows superior lithium storage capacity with 1202 mAh g −1 after 100 cycles at 100 mA g −1 and high-rate performance with 543 mAh g −1 even at 2000 mA g −1 . The corresponding lithium-ion capacitor with NiFe-LDH/rGO anode and mesoporous carbon microsphere cathode exhibits high energy density and power density simultaneously, with 133 Wh kg −1 at 25 W kg −1 and 4016 W kg −1 at 58 Wh kg −1 , showing the great potential for highperformance hybrid energy storage systems.