Three-Dimensional Ni-MOF as a High-Performance Supercapacitor Anode Material; Experimental and Theoretical Insight

A three-dimensional (3D) Ni-MOF of the formula [Ni(C 4 H 4 N 2 )(CHO 2 ) 2 ] n, has been reported, which shows a capacitance of 2150 F/g at a current density of 1A/g in a three-electrode setup (5.0 M KOH). Post-mortem analysis of the sample after three-electrode measurements revealed the bias-induced transformation of Ni-MOF to Ni(OH) 2, which has organic constituents intercalated within the sample exhibiting better storage performance than bulk Ni(OH) 2 . Afterward, the synthesized MOF and reduced graphene (rGO) were used as the anode and cathode electrode material, respectively, and a two-electrode asymmetric supercapacitor device (ASC) setup was designed that exhibited a capacitance of 125 F/g (at 0.2 A/g) with a high energy density of 50.17 Wh/kg at a power density of 335.1 W/kg. The ASC further has a very high reversibility (97.9% Coulombic efficiency) and cyclic stability (94%) after 5000 constant charge–discharge cycles. Its applicability was also demonstrated by running a digital watch. Using sophisticated density functional theory simulations, the electronic properties, diffusion energy barrier for the electrolytic ions (K + ), and quantum capacitance for the Ni(OH) 2 electrode have been reported. The lower diffusion energy barrier (0.275 eV) and higher quantum capacitance (1150 μF/cm 2 ) are attributed to the higher charge storage performance of the Ni-MOF-transformed Ni(OH) 2 electrode as observed in the experiment.