Promoting Active Sites for Hydrogen Evolution in MoSe2 via Transition-Metal Doping

过电位 空位缺陷 材料科学 过渡金属 兴奋剂 化学物理 催化作用 密度泛函理论 结晶学 金属 掺杂剂 无机化学 化学 电化学 物理化学 计算化学 冶金 光电子学 有机化学 生物化学 电极
作者
Akash Jain,Maya Bar‐Sadan,Ashwin Ramasubramaniam
出处
期刊:Journal of Physical Chemistry C [American Chemical Society]
卷期号:124 (23): 12324-12336 被引量:44
标识
DOI:10.1021/acs.jpcc.0c00013
摘要

Molybdenum diselenide (MoSe2)—a transition-metal dichalcogenide—is a promising nonprecious metal catalyst for the hydrogen evolution reaction (HER). However, practical application of MoSe2 for electrocatalytic HER is hindered by its poor electrical conductivity, its high overpotential, and the limited number of active sites. Specifically, while the edges of MoSe2 are highly active for HER, the basal plane, which constitutes most of the catalyst surface, is inert toward HER. Although prior studies have focused on improving the activity of MoSe2 either by promoting the formation of highly active basal-plane Se vacancies or by substitutional doping of metal atoms, the interaction between dopants and Se vacancies—whether beneficial or detrimental toward HER—has not been fully understood. Here, we employ density functional theory calculations to study the interplay between prototypical transition metal (TM) dopants (Mn, Fe, Co, and Ni) and Se vacancies, and the consequent influence on hydrogen adsorption (a descriptor of HER activity in acidic media) at basal planes, edges, and Se vacancy sites. We correlate trends in the free energies of hydrogen adsorption and Se vacancy formation with changes in the electronic structure of MoSe2 upon TM doping as well as structural changes arising because of TM dopant atoms. Broadly, our studies show that the studied electron-rich TM dopants favorably modify the electronic structure of MoSe2 basal planes toward HER and, additionally, electrochemical generation of Se vacancies becomes more facile on the doped basal plane and edges at smaller cathodic potentials. These newly formed Se vacancies are typically highly active toward HER and substitutional doping can be viewed as an avenue for defect-mediated activation of MoSe2.
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