Ternary MOF-Based Redox Active Sites Enabled 3D-on-2D Nanoarchitectured Battery-Type Electrodes for High-Energy-Density Supercapatteries

Designing rationally combined metal-organic frameworks (MOFs) with multifunctional nanogeometries is of significant research interest to enable the electrochemical properties in advanced energy storage devices. Herein, we explored a new class of binderfree dual-layered Ni-Co-Mn-based MOFs (NCM-based MOFs) with three-dimensional (3D)-on-2D nanoarchitectures through a polarityinduced solution-phase method for high-performance supercapatteries. The hierarchical NCM-based MOFs having grown on nickel foam exhibit a battery-type charge storage mechanism with superior areal capacity (1311.4 mu Ah -cm-2 at 5 mA cm-2), good rate capability (61.8%; 811.67 mu Ah -cm-2 at 50 mA cm-2), and an excellent cycling durability. The superior charge storage properties are ascribed to the synergistic features, higher accessible active sites of dual-layered nanogeometries, and exalted redox chemistry of multi metallic guest species, respectively. The bilayered NCM-based MOFs are further employed as a battery-type electrode for the fabrication of supercapattery paradigm with biomass-derived nitrogen/oxygen doped porous carbon as a negative electrode, which demonstrates excellent capacity of 1.6 mAh -cm-2 along with high energy and power densities of 1.21 mWh -cm-2 and 32.49 mW -cm-2, respectively. Following, the MOF-based supercapattery was further assembled with a renewable solar power harvester to use as a self-charging station for various portable electronic applications.

Automated summary

Designing rational combined metal-organic frameworks (MOFs) with multifunctional nanogeometries is crucial for enhancing the electrochemical properties in energy storage devices. In this study, a new class of dual-layered Ni-Co-Mn-based MOFs with high-performance capabilities was explored, showcasing superior charge storage properties and excellent cycling durability. These MOFs were further used as electrodes for supercapattery devices, achieving high energy and power densities when combined with biomass-derived nitrogen/oxygen doped porous carbon as the negative electrode.