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1.
Nanomaterials (Basel) ; 13(23)2023 Dec 04.
Artigo em Inglês | MEDLINE | ID: mdl-38063772

RESUMO

Double perovskites are known for their special structures which can be utilized as catalyst electrode materials for electrochemical water splitting to generate carbon-neutral hydrogen energy. In this work, we prepared lanthanide series metal-doped double perovskites at the M site such as M2NiMnO6 (where M = Eu, Gd, Tb) using the solid-state reaction method, and they were investigated for an oxygen evolution reaction (OER) study in an alkaline medium. It is revealed that the catalyst with a configuration of Tb2NiMnO6 has outstanding OER properties such as a low overpotential of 288 mV to achieve a current density of 10 mAcm-2, a lower Tafel slope of 38.76 mVdec-1, and a long cycling stability over 100 h of continuous operation. A-site doping causes an alteration in the oxidation or valence states of the NiMn cations, their porosity, and the oxygen vacancies. This is evidenced in terms of the Mn4+/Mn3+ ratio modifying electronic properties and the surface which facilitates the OER properties of the catalyst. This is discussed using electrochemical impedance spectroscopy (EIS) and electrochemical surface area (ECSA) of the catalysts. The proposed work is promising for the synthesis and utilization of future catalyst electrodes for high-performance electrochemical water splitting.

2.
Membranes (Basel) ; 13(9)2023 Aug 22.
Artigo em Inglês | MEDLINE | ID: mdl-37755170

RESUMO

Layered double hydroxides (LDHs) have gained vast importance as an electrocatalyst for water electrolysis to produce carbon-neutral and clean hydrogen energy. In this work, we demonstrated the fabrication of nano-flake-like NiMn LDH thin film electrodes onto porous membrane-like Ni-foam by using a simple and cost-effective electrodeposition method for oxygen evolution reaction (OER). Various Ni1-xMnx LDH (where x = 0.15, 0.25, 0.35, 0.50 and 0.75) thin film electrodes are utilized to achieve the optimal catalyst for an efficient and sustainable OER process. The various composition-dependent surface morphologies and porous-membrane-like structure provided the high electrochemical surface area along with abundant active sites facilitating the OER. The optimized catalyst referred to as Ni0.65Mn0.35 showed excellent OER properties with an ultralow overpotential of 253 mV at a current density of 50 mAcm-2, which outperforms other state-of-the art catalysts reported in the literature. The relatively low Tafel slope of 130 mV dec-1 indicates faster and more favorable reaction kinetics for OER. Moreover, Ni0.65Mn0.35 exhibits excellent durability over continuous operation of 20 h, indicating the great sustainability of the catalyst in an alkaline medium. This study provides knowledge for the fabrication and optimization of the OER catalyst electrode for water electrolysis.

3.
Dalton Trans ; 52(39): 13852-13857, 2023 Oct 10.
Artigo em Inglês | MEDLINE | ID: mdl-37772345

RESUMO

The doping of metal-organic frameworks (MOFs) with metal-ions has emerged as a powerful strategy for enhancing their catalytic performance. Doping allows for the tailoring of the electronic structure and local coordination environment of MOFs, thus imparting on them unique properties and enhanced functionalities. This frontier article discusses the impact of metal-ion doping on the electronic structure and local coordination of MOFs, highlighting the effects on their electrocatalytic properties in relation to the oxygen evolution reaction (OER). The fundamental mechanisms underlying these modifications are explored, while recent advances, challenges, and prospects in the field are discussed. In addition, experimental techniques that can be applied to tackle the realization of effective metal-ion doping of MOFs are also noted briefly.

4.
Dalton Trans ; 52(34): 12020-12029, 2023 Aug 29.
Artigo em Inglês | MEDLINE | ID: mdl-37581273

RESUMO

Operating temperatures considerably influence the energy storage mechanism of the anode of Li-ion batteries (LiBs). This effect must be comprehensively studied to facilitate the effective integration of LiBs in practical applications and battery management. In this study, we fabricated a novel anode material, i.e., copper-iron-tin-sulphide (Cu2FeSnS4, CFTS), and investigated the corresponding LiB performance at operating temperatures ranging from 10 °C to 55 °C. The CFTS anode exhibited a discharge capacity of 283.1 mA h g-1 at room temperature (25 °C), which stabilized to 174.0 mA h g-1 in repeated cycles tested at a current density of 0.1 A g-1. The discharge capacity at higher operating temperatures, such as 40 °C and 55 °C, is found to be 209.3 and 230.0 mA h g-1 respectively. In contrast, the discharge capacity decreased to 36.2 mA h g-1 when the temperature decreased to 10 °C. Electrothermal impedance spectroscopy was performed to determine the rate of chemical reactions, mobility of active species, and change in internal resistance at different operating temperatures. In terms of the cycle life, CFTS exhibited outstanding cycling stability for more than 500 charge/discharge cycles, with a 146% capacity retention and more than 80% coulombic efficiency. The electrochemical investigation revealed that the charge storage in the CFTS anode is attributable to capacitive-type and diffusion-controlled mechanisms.

5.
Dalton Trans ; 52(31): 10933-10941, 2023 Aug 08.
Artigo em Inglês | MEDLINE | ID: mdl-37490008

RESUMO

This work reports a promising and sustainable method for valorization of abundantly available biomass feedstocks to overcome the thermodynamic high energy barrier of the OER via glucose electrolysis as a proxy anodic reaction, thereby driving the energy-efficient water splitting for green hydrogen generation. For this, a robust and efficient MIL-88B(Fe) based electrocatalyst is engineered via Cu doping. The ultrasonically prepared Cu-doped@ MIL-88B ink when drop-cast on nickel foam (NF) produces thin nano-porous 2D-sheet like films having a thickness of ca. 300 nm and demonstrates an excellent glucose oxidation reaction (GOR) with a lower potential of 1.35 V versus RHE at 10 mA cm-2. In addition, this electrode shows outstanding long-term electrochemical durability for 50 h and exhibits the maximum GOR current load of 350 mA cm-2 at 1.48 V vs. RHE, while the pristine MIL-88B based electrode exhibits a current load of only 180 mA cm-2 at the same potential bias. The remarkably higher current density after doping indicates an accelerated GOR, which is ascribed to the electronic structure modulation of the Fe nodes by Cu, thereby enhancing the active sites and charge transport characteristics of the frameworks. Most importantly, the MOF-based electrodes demonstrate the occurrence of the GOR prior to the OER at a large potential difference, hence assisting the energy-efficient water splitting for green hydrogen production.

6.
Dalton Trans ; 51(38): 14535-14544, 2022 Oct 04.
Artigo em Inglês | MEDLINE | ID: mdl-36073276

RESUMO

In everyday life, superior lithium-ion batteries (LIBs), with fast charging ability, have become valuable assets. The LIB performance of an anode composite copper cobalt tin sulphide (Cu2CoSnS4; CCTS) electrode, which was fabricated using a simple and easy hydrothermal method, was investigated. The electrochemical charge storage performance of the CCTS anode demonstrated sustainability, high-rate capability and efficiency. The CCTS anode exhibited a first discharge capacity of 914.5 mA h g-1 and an average specific capacity of 198.7 mA h g-1 in consecutive cycles at a current density of 0.1 A g-1. It had a capacity retention of ∼62.0% and a coulombic efficiency of more than 83% after over 100 cycles, demonstrating its excellent cycling performance and reversibility. It can be an alternative anode to other established electrode materials for real battery applications.

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