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1.
J Colloid Interface Sci ; 652(Pt B): 1665-1672, 2023 Dec 15.
Article in English | MEDLINE | ID: mdl-37666198

ABSTRACT

The rational design of electrocatalysts with exceptional performance and durability for hydrogen production in alkaline medium is a formidable challenge. In this study, we have developed in-situ activated ruthenium nanoparticles dispersed on Ni3N nanosheets, forming a bifunctional electrocatalyst for hydrogen evolution and urea oxidation. The results of experimental analysis and theoretical calculations reveal that the enhanced hydrogen evolution reaction (HER) performance of O-Ru-Ni3N stems primarily from the optimized hydrogen adsorption and hydroxyl adsorption on Ru sites. The O-Ru-Ni3N on nickel foam (NF) electrode exhibits excellent HER performance, requiring only 29 mV to reach 10 mA cm-2 in an alkaline medium. Notably, when this O-Ru-Ni3N/NF catalyst is employed for both HER and urea oxidation reaction (UOR) to create an integrated H2 production system, a current density of 50 mA cm-2 can be generated at the cell voltage of 1.41 V. This report introduces an energy-efficient catalyst for hydrogen production and proposes a viable strategy for anodic activation in energy chemistry.

2.
Inorg Chem ; 62(6): 2784-2792, 2023 Feb 13.
Article in English | MEDLINE | ID: mdl-36705969

ABSTRACT

Efficient electrocatalysts require not only a tunable electronic structure but also great active site accessibility and favorable mass transfer. Here, a two-dimensional/three-dimensional (2D/3D) hierarchical electrocatalyst consisting of Co(OH)2-CeO2 nanosheet-decorated Co dendrites is proposed, named as Co(OH)2-CeO2/Co. Based on the strong electronic interaction of the Co(OH)2-CeO2 heterojunction, the electronic structure of the Co site is optimized, which facilitates the adsorption of intermediates and the dissociation of H2O. Moreover, the open 2D/3D structure formed by introducing the Co substrate further reduces the accumulation of heterogeneous nanosheets and promotes the radial diffusion of the electrolyte, significantly improving the utilization of active sites and shortening the electron transfer pathway. In addition, the superhydrophilic/superaerophobic interface achieved by constructing the hierarchical micro-nanostructure is beneficial to electrolyte infiltration and bubble desorption, thus ensuring favorable mass transfer. Therefore, Co(OH)2-CeO2/Co exhibits an excellent overall water-splitting activity in alkaline solution.

3.
J Colloid Interface Sci ; 618: 196-205, 2022 Jul 15.
Article in English | MEDLINE | ID: mdl-35338926

ABSTRACT

The development of highly efficient oxygen evolution reaction (OER) and urea oxidation reaction (UOR) electrocatalysts with abundant resources is necessary for green hydrogen production. Ni-based compounds have received attention as the most promising earth-abundant electrocatalysts for OER and UOR, whereas some compounds in this main group, e.g., nickel selenides and tellurides, have received little attention. Herein, we demonstrate the interfacial engineered Ni0.85Se/NiTe array on Ni foam as a highly efficient catalyst for the OER, which exhibits an overpotential of 200 mV to obtain a current density of 10 mA cm-2 in alkaline solutions. Meanwhile, it exhibits a low potential of 1.301 V for the UOR at a current density of 100 mA cm-2. In particular, it even has the potential to be used in methanol oxidation reaction and ethanol oxidation reaction. The vertical NiTe array not only serves as the conductive substrate for highly improving the mass loading of Ni0.85Se, but also triggers the strong electron interaction between two components, leading to increased adsorption sites available for the intermediates formed in the OER and UOR on the Ni0.85Se surface. This study provides a broad avenue to construct hierarchical nanostructures as outstanding electrocatalysts for efficient OER and UOR.

4.
Nanoscale ; 13(42): 17846-17853, 2021 Nov 04.
Article in English | MEDLINE | ID: mdl-34668912

ABSTRACT

Electrochemical water splitting is widely studied in the hope of solving environmental deterioration and energy shortage. The design of inexpensive metal catalysts exhibiting desired catalytic performance and durable stability for efficient oxygen evolution is the pursuit of sustainable and clean energy fields. Herein, a three-dimensional (3D) flower-like NiSe2 primary structure, modified with highly dispersed CuSe2 nanoclusters as the secondary structure, is obtained by regulating the growth trend of the nanosheets. Benefiting from the metallicity of selenides and the formation of a heterogeneous interface, NiSe2@CuSe2/NF shows comparable performance toward the oxygen evolution reaction (OER) in an alkaline environment. Upon regulating the synthesis conditions, the catalyst exhibits its optimal performance with ultralow overpotential for the OER when the Ni/Cu molar ratio is 1 : 0.2 and the hydrothermal temperature and hydrothermal time are 200 °C and 6 h, respectively. It provides a current density of 10 mA cm-2 when a potential of 201 mV is applied without iR compensation. In this work, the hierarchical heterostructures of NiSe2 and CuSe2 are synthesized, which exhibit high electrocatalytic activity towards the oxygen evolution reaction and provides a new possibility for the extensive application of copper-based compounds in advanced energy fields.

5.
Nanoscale ; 12(38): 19992-20001, 2020 Oct 08.
Article in English | MEDLINE | ID: mdl-32996530

ABSTRACT

The design of Earth-abundant and cost-effective electrocatalysts for highly active and stable electrochemical water splitting in practical production is the primary demand. Herein, bimetallic oxides anchored to three-dimensional (3D) porous conductive nickel foam (NF) are constructed using a simple in situ hydrothermal method for efficient overall water splitting. The vertically aligned Mn3O4/Fe2O3 heterojunction nanosheets have synergy between hierarchical metal oxides and heterogeneous interface, and show excellent performance toward the oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) in an alkaline environment. By adjusting the molar ratio of Fe : Mn, the morphology, composition and electronic structure of MnFeO-NF-x composites (x represents the ratio of Fe : Mn) can be adjusted to exhibit diverse catalytic activities. In particular, MnFeO-NF-0.4 (0.4 indicates the Fe : Mn ratio of 0.4 : 1) and MnFeO-NF-0.8 display outstanding performance with ultralow overpotentials of 157 mV for the OER and 64 mV for the HER to achieve a current density of 10 mA cm-2, respectively. Furthermore, MnFeO-NF-0.4 and MnFeO-NF-0.8 are assembled into a water splitting electrolyzer, which can reach a current density of 10 mA cm-2 with a low voltage of 1.59 V. Interestingly, Mn-M (M = Co, Ni, and Mo) products can be obtained easily by using different metal salts, indicating the universality of the current one-pot hydrothermal method.

6.
Chem Commun (Camb) ; 56(82): 12339-12342, 2020 Oct 21.
Article in English | MEDLINE | ID: mdl-32930292

ABSTRACT

Herein, we have synthesized successfully a three-dimensional/two dimensional (3D/2D) core-shell Cu2O@Fe-Ni3S2 nanoflower on copper foam at room temperature. Remarkably, by virtue of rich active sites and vacancies, large surface area, high conductivity and close contact with the electrolyte, the Cu2O@Fe-Ni3S2 catalyst exhibits superior stability and oxygen evolution reaction performance.

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