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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:Biowaste eggshell can be used as a cathode while in its calcined form and it is found to be suitable as an anode in an electrochemical cell. This not only enables energy to be stored reversibly but also achieves waste management and sustainability goals by redirecting material away from landfill. Biowaste eggshell comprises 94% calcium carbonate (CaCO3; calcite), an attractive divalent ion source as a viable option for energy storage. X-ray diffraction and electron microscopy coupled with energy dispersive analyses of the calcined (thermally decomposed) biowaste eggshell show that CaO has been formed and the reaction is topotactic. Field emission scanning electron microscopy (FESEM) images of the textural relationship show that the thermal decomposition of calcite resulted in a change in morphology. High-resolution XPS spectra of the C 1s core level from the CaCO3 and CaO shows that there is a chemical difference in the carbon environments and the total atomic fraction of Ca for each sample with that of carbonate and oxygen varies. In a three-electrode configuration, a working electrode of CaCO3 is found to be electrochemically active in the positive region, whereas a CaO electrode is active in the negative region. This indicates the potential use of eggshell-derived materials for both cathode and anode. Both the electrodes exhibited a quasi-box-shaped potentiostatic curve implying a capacitor-type behaviour. The CaCO3 cathode possesses a modest discharge capacitance of 10 F g-1 but the CaO anode showed excellent capacitance value of 47.5 F g-1. The CaO electrode in both positive and negative regions, at a current density of 0.15 A g-1 exhibited 55 F g-1 with a retention of nearly 100% after 1000 cycles. At a very low sweep rate of 0.5 mV s-1, the CaO electrode showed typical redox-type behaviour with well-defined peaks illustrating battery-type behaviour. The outcome of the calcite/CaO transformation, exhibiting technological importance for energy storage applications, may help to re-evaluate biowaste before throwing it away. The current work explores the viability of eggshell derived materials as a cathode/anode for use in batteries and capacitors.

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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