High-energy-density zinc ion capacitors based on 3D porous free-standing defect-reduced graphene oxide hydrogel cathodes

Abstract

Zinc ion capacitors (ZICs) have shown potential for breaking the energy density ceiling of traditional supercapacitors (SCs) via appropriate device design. Nevertheless, a significant challenge remains in advancing ZIC positive electrode materials with excellent conductivity, high specific capacitance, and reliable cycle stability. A highly attractive option for carbon-based electrode materials is reduced graphene oxide (RGO) due to its vast specific surface area, prominent porosity, and 3D cross-linked frame. However, the tight stacking of RGO sheets driven by van der Waals forces can restrict active sites, decrease specific capacitance, and elevate electrochemical impedance. To overcome these challenges, 3D defective RGO (DRGO) hydrogels were prepared by a metal Co cocatalytic gasification reaction. This method produced mesoporous defects on the surface of RGO hydrogels via a low-temperature hydrothermal self-assembly strategy. The surface of the layer has a wide and uniform distribution, which can offer abundant redox active sites, rich ion transfer channels, and fast reaction kinetics. In this work, 3D DRGO//Zn exhibited a wide operating window (0–1.8 V), high specific capacitance (189.39 F g⁻¹ at 1 A g⁻¹), outstanding energy density (85.23 W h kg⁻¹ at 960.31 W kg⁻¹; 52.36 W h kg⁻¹ at ¹7454.87 W kg⁻¹), and persistent cycling life (98.86% initial capacitance retention after 10 000 cycles at 10 A g⁻¹). This study emphasizes the device design of ZIC and promising prospects of using 3D DRGO hydrogel as a feasible positive electrode for ZIC.