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

Abstract

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 binder-free dual-layered Ni–Co–Mn-based MOFs (NCM-based MOFs) with three-dimensional (3D)-on-2D nanoarchitectures through a polarity-induced 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 μAh cm−2 at 5 mA cm−2), good rate capability (61.8%; 811.67 μAh 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.

CuCo LDHs Coated CuCoTe Honeycomb‐Like Nanosheets as a Novel Anode Material for Hybrid Supercapacitors

“…Further, the power law and its modified versions were utilized to calculate the exact contributions of each type. [ 47 ] where k 1 and k 2 are the parameters deductible from the slope and intercept of the linear curves shown in Figure 6h. The obtained k 1 and k 2 values are substituted in Equation () or () and the capacitive ( k 1 υ ) and diffusive ( k 2 υ ) contributions are calculated as depicted in Figure 6i.…”

An Amorphous–Crystalline Nanosheet Arrays Structure for Ultrahigh Electrochemical Performance Supercapattery

“…Figure 3a There are a pair of obvious redox peaks, confirming the existence of battery-type electrochemical behavior. [3,10] During the process, the redox reaction of the MoO 3 -Ni 3 S 2 /NF-0.5 electrode will proceed as follows: [32,33] Ni S 3OH Ni S OH 3e…”

“…Based on the above, hybrid supercapacitors (HSCs) also called supercapattery with battery-type positive electrode as the energy source and electric double-layer capacitor negative electrode as the power source have been designed, it combines the dual advantages of high power density of traditional SCs and high energy density of batteries. [7][8][9][10] Further, the electrochemical properties of the HSCs are mainly determined by the battery-type electrode, so selecting suitable electrode materials or optimizing the electrode structure is essential for obtaining high-performance hybrid devices.Transition metal oxides and sulfides have become the most widely studied battery-type electrodes due to their remarkable electrochemical activity and high specific capacity. [11][12][13] For example, Chen et al reported the self-supported Ni 3 S 2 nanosheet arrays by a two-step method.…”

Hierarchical NiCo / NiO / NiCo 2 O 4 composite formation by solvothermal reaction as a potential electrode material for hydrogen evolutions and asymmetric supercapacitors

“…The GCD profiles show the almost symmetric shape and non-linear behavior, demonstrating the sturdy battery-type redox reaction, highly reversible, and possess a low degree of polarization. 60,61 The C s of electrode materials were calculated using the following equation based on the integration of the discharge curve, 59,60 as presented in Figure 6H.…”