二维M2X2( M:Mo、W和X:F、Cl )析氢和析氧反应的电催化性能

doi:10.3969/j.issn.1000-1565.2024.06.005

摘要/Abstract

摘要： 以剥离密排六方结构(HCP)的块状金属,形成单层金属薄膜为切入点,通过用卤素原子钝化中间金属层的方法,形成了一类稳定的ABAB堆叠的金属卤素化合物.对比了*O中吸附O原子和不吸附O原子的Mo-d投影态密度图,期望揭示电子排布、成键状态与材料催化性能之间的关联.电子结构计算表明Mo₂X₂和W₂X₂具有很好的导电性.通过与过渡金属二硫化物(MoS₂)类比,将缺陷工程(卤素原子空位)引入活性位点,然后计算了其在四电子转移析氧反应中的反应能垒,发现它们具有良好的催化性能,其中,W₂Cl₂的析氧催化性能最好,过电位仅有1.95 V.最后,通过详细分析电子、轨道之间耦合作用,给出了清晰的物理图像.

关键词: 电子结构, 电催化析氧反应, 密度泛函理论

Abstract: Starting from stripping the bulk metal of the hexagonal close-packed( HCP )crystal structure and forming a single-layer metal film, a stable ABAB-stacked metal halide compound was formed by passivating the intermediate metal layer with halogen atoms. The Mo-d projected density of states of adsorbed O atoms and non-adsorbed O atoms in *O are compared, and it is expected to reveal the relationship between electron arrangement, bonding state and catalytic performance of materials. Electronic structure calculations show that Mo₂X₂ and W₂X₂ have good electrical conductivity. By analogy with transition metal disulfides( MoS₂ ), defect engineering( halogen atom vacancies )is introduced into active sites, and then their reaction energy barriers in the four-electron transfer oxygen evolution reaction are calculated. It is found that they have good catalytic performance. Among them, W₂Cl₂ has the best oxygen evolution catalytic performance, and the overpotential is only 1.95 V. Finally, a clear physical image is given by analyzing the coupling between electrons and orbits in detail.

Key words: Electronic structure, Electrocatalytic oxygen evolution reaction, Density functional theory

中图分类号:

O469

侯懿娜,王博静,王瑞宁. 二维M₂X₂( M:Mo、W和X:F、Cl )析氢和析氧反应的电催化性能[J]. 河北大学学报(自然科学版), 2024, 44(6): 602-611.

HOU Yina, WANG Bojing, WANG Ruining. Electrocatalytic properties of two-dimensional M₂X₂( M: Mo、W and X: F、Cl )for hydrogen and oxygen evolution reactions[J]. Journal of Hebei University(Natural Science Edition), 2024, 44(6): 602-611.

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二维M₂X₂( M:Mo、W和X:F、Cl )析氢和析氧反应的电催化性能

Electrocatalytic properties of two-dimensional M₂X₂( M: Mo、W and X: F、Cl )for hydrogen and oxygen evolution reactions

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