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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.

SUBMITTER: Nagaraju G

PROVIDER: S-EPMC8187485 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Project description:The surface properties of porous carbonaceous electrodes govern the performance, durability, and ultimately the cost of redox flow batteries (RFBs). State-of-the-art carbon fiber-based electrode interfaces suffer from limited kinetic activity and incomplete wettability, fundamentally limiting the performance. Surface treatments for electrodes such as thermal and acid activation are a common practice to make them more suitable for aqueous RFBs; however, these treatments offer limited control over the desired functional properties. Here, we propose, for the first time, electrografting as a facile, rapid, and versatile technique to enable task-specific functionalization of porous carbonaceous electrodes for use in RFBs. Electrografting allows covalent attachment of organic molecules on conductive substrates upon application of an electrochemical driving force, and the vast library of available organic molecules can unlock a broad range of desired functional properties. To showcase the potential of electrografting for RFBs, we elect to investigate taurine, an amine with a highly hydrophilic sulfonic acid tail. Oxidative electrografting with cyclic voltammetry allows covalent attachment of taurine through the amine group to the fiber surface, resulting in taurine-functionalized carbon cloth electrodes. In situ polarization and impedance spectroscopy in single-electrolyte flow cells reveal that taurine-treated cloth electrodes result in 40% lower charge transfer and 25% lower mass transfer resistances than off-the-shelf cloth electrodes. We find that taurine-treated electrode interfaces promote faster Fe3+ reduction reaction kinetics as the electrochemical surface area normalized current densities are 2-fold and 4-fold higher than oxidized and untreated glassy carbon surfaces, respectively. Improved mass transfer of taurine-treated electrodes is attributed to their superior wettability, as revealed by operando neutron radiography within a flow cell setup. Through demonstrating promising results for aqueous systems with the model molecule taurine, this work aims to bring forth electrografting as a facile technique to tailor electrode surfaces for other RFB chemistries and electrochemical technologies.

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

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