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Advanced Carbon-Nickel Sulfide Hybrid Nanostructures: Extending the Limits of Battery-Type Electrodes for Redox-Based Supercapacitor Applications.

ABSTRACT: Transition-metal sulfides combined with conductive carbon nanostructures are considered promising electrode materials for redox-based supercapacitors due to their high specific capacity. However, the low rate capability of these electrodes, still considered "battery-type" electrodes, presents an obstacle for general use. In this work, we demonstrate a successful and fast fabrication process of metal sulfide-carbon nanostructures ideal for charge-storage electrodes with ultra-high capacity and outstanding rate capability. The novel hybrid binder-free electrode material consists of a vertically aligned carbon nanotube (VCN), terminated by a nanosized single-crystal metallic Ni grain; Ni is covered by a nickel nitride (Ni₃N) interlayer and topped by trinickel disulfide (Ni₃S₂, heazlewoodite). Thus, the electrode is formed by a Ni₃S₂/Ni₃N/Ni@NVCN architecture with a unique broccoli-like morphology. Electrochemical measurements show that these hybrid binder-free electrodes exhibit one of the best electrochemical performances compared to the other reported Ni₃S₂-based electrodes, evidencing an ultra-high specific capacity (856.3 C g^-1 at 3 A g^-1), outstanding rate capability (77.2% retention at 13 A g^-1), and excellent cycling stability (83% retention after 4000 cycles at 13 A g^-1). The remarkable electrochemical performance of the binder-free Ni₃S₂/Ni₃N/Ni@NVCN electrodes is a significant step forward, improving rate capability and capacity for redox-based supercapacitor applications.

SUBMITTER: Santhosh NM

PROVIDER: S-EPMC8289178 | 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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Advanced Carbon-Nickel Sulfide Hybrid Nanostructures: Extending the Limits of Battery-Type Electrodes for Redox-Based Supercapacitor Applications.

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