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用于高效析氢的钼/硒基异质结构催化剂:离子溶解和再聚合对催化性能的影响

Molybdenum/selenium based heterostructure catalyst for efficient hydrogen evolution: Effects of ionic dissolution and repolymerization on catalytic performance.

作者信息

Yang Mameng, Bao Weiwei, Zhang Junjun, Ai Taotao, Han Jie, Li Yan, Liu Jiangying, Zhang Pengfei, Feng Liangliang

机构信息

National and Local Joint Engineering Laboratory for Slag Comprehensive Utilization and Environmental Technology, School of Materials Science and Engineering, Shaanxi University of Technology, Hanzhong 723000, Shaanxi, PR China.

National and Local Joint Engineering Laboratory for Slag Comprehensive Utilization and Environmental Technology, School of Materials Science and Engineering, Shaanxi University of Technology, Hanzhong 723000, Shaanxi, PR China.

出版信息

J Colloid Interface Sci. 2024 Mar 15;658:32-42. doi: 10.1016/j.jcis.2023.12.033. Epub 2023 Dec 9.

Abstract

Transition metal chalcogenides (TMCs) are recognized as highly efficient electrocatalysts and have wide applications in the field of hydrogen production by electrolysis of water, but the real catalytic substances and catalytic processes of these catalysts are not clear. The species evolution of Mo and Se during alkaline hydrogen evolution was investigated by constructing MoSe@CoSe heterostructure. The real-time evolution of Mo and Se in MoSe@CoSe was monitored using in situ Raman spectroscopy to determine the origin of the activity. Mo and Se in MoSe@CoSe were dissolved in the form of MoO and SeO, respectively, and subsequently re-adsorbed and polymerized on the electrode surface to form new species MoO and SeO. Theoretical calculations show that adsorption of MoO and SeO can significantly enhance the HER catalytic activity of Co(OH). The addition of additional MoO and SeO to the electrolyte with Co(OH) electrodes both enhances its HER activity and promotes its durability. This study helps to deepen our insight into mechanisms involved in the structural changes of catalyst surfaces and offers a logical basis for revealing the mechanism of the influence of species evolution on catalytic performance.

摘要

过渡金属硫族化合物(TMCs)被认为是高效的电催化剂,在水电解制氢领域有着广泛的应用,但这些催化剂的实际催化物质和催化过程尚不清楚。通过构建MoSe@CoSe异质结构,研究了碱性析氢过程中Mo和Se的物种演变。利用原位拉曼光谱监测MoSe@CoSe中Mo和Se的实时演变,以确定活性的来源。MoSe@CoSe中的Mo和Se分别以MoO和SeO的形式溶解,随后重新吸附并在电极表面聚合形成新的物种MoO和SeO。理论计算表明,MoO和SeO的吸附可以显著提高Co(OH)的析氢催化活性。在含有Co(OH)电极的电解液中添加额外的MoO和SeO,既能提高其析氢活性,又能提高其耐久性。这项研究有助于加深我们对催化剂表面结构变化所涉及机制的理解,并为揭示物种演变对催化性能影响的机制提供了合理依据。

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