Nonmetal doping is an efficient approach to activate inert MoS₂ basal plane, which converts MoS₂ into an electrocatalyst for the hydrogen evolution reaction (HER). However, the trial-and-error approach through experimental attempt is still a common practice to search for suitable nonmetal dopants. In this work, we employ density functional theory (DFT) and microkinetic model to assess alkaline HER activity of nonmetal-modified MoS₂(0 0 1), which show strong variation in the degree of activation by single- or double-dopants across nonmetal element series (B, C, N, P, O, S, Se and Te). To assist the screening of nonmetal dopants to active MoS₂ basal plane, a structural descriptor-based prediction model is constructed. It demonstrates that the activation effect of nonmetal dopant is achieved through the adjustment of valence electron occupancy of reaction center, which tunes the adsorption energy of atomic hydrogen and hydroxide radical, and accordingly reaction kinetic for alkaline HER. The structural descriptor-based prediction model reproduce the activity trend among non-metallic doped MoS₂ from available experimental references. In addition, we screened out MoS₂ modified by BTe and BSe double dopants with lower overpotential than reported nonmetal-modified MoS₂ systems. This work gives a deep insight into activation mechanism of nonmetal dopant for MoS₂, and provides an efficient screening strategy for future catalyst design of transition metal dichalcogenides.

非金属掺杂是激活惰性 MoS ₂基面​​的有效方法，可将 MoS ₂转化为析氢反应 (HER) 的电催化剂。然而，通过实验尝试的反复试验方法仍然是寻找合适的非金属掺杂剂的常见做法。在这项工作中，我们采用密度泛函理论 (DFT) 和微动力学模型来评估非金属改性 MoS ₂ (0  0  1) 的碱性 HER 活性，这表明单掺杂剂或双掺杂剂在非金属中的活化程度存在很大差异元素系列（B、C、N、P、O、S、Se 和 Te）。协助筛选非金属掺杂剂到活性 MoS ₂基面，构建基于结构描述符的预测模型。这表明非金属掺杂剂的活化作用是通过调节反应中心的价电子占据来实现的，从而调节原子氢和氢氧根的吸附能，从而调节碱性HER的反应动力学。基于结构描述符的预测模型从可用的实验参考中再现了非金属掺杂 MoS _{2之间的活性趋势。}此外，我们筛选出由BTe和BSe双掺杂剂改性的MoS ₂，其过电势低于报道的非金属改性MoS ₂系统。这项工作深入了解了非金属掺杂剂对 MoS _{2的活化机制}，并为未来过渡金属二硫属化物的催化剂设计提供了一种有效的筛选策略。