Platinum diselenide (PtSe₂) has been successfully fabricated with a hope of catalytic applications. However, the active sites of pristine PtSe₂ are only located at the edges while the sites in basal plane are largely inactive. To change such situation, in this study we introduce Pd dopant and vacancies to activate the basal plane for hydrogen evolution reaction (HER). Based on systematic density functional theory calculations, we find that Pd doping reduces the band gap and enhances the catalytic ability, and the divacancy sites (V_Se2 and V_Pt2) in pristine PtSe₂ monolayer and the monovacancy sites (V_Se, V_Pd) as well as the divacancy sites (V_Pt2, V_PdPt) in PdPtSe₄ monolayer significantly improve the catalytic activities comparable to that of Pt(1 1 1). A band-center model is applied to better understand the difference in HER activities, where the chemical bond energies of H (ΔG₁) show an approximately linear relationship with the energy of d /p level of Pt/ Se. The strategy proposed here would be applicable to other two-dimensional materials.

二硒化铂（PtSe ₂）已经成功地制备，希望能被催化应用。然而，原始PtSe ₂的活性位点仅位于边缘，而基面上的活性位点基本上没有活性。为了改变这种情况，在本研究中，我们引入Pd掺杂剂和空位来激活氢释放反应（HER）的基面。基于系统的密度泛函理论计算，我们发现Pd掺杂减少了带隙并增强了催化能力，原始PtSe ₂单层中的空位（V _Se2和V _Pt2）和单空位（V _Se，V _Pd）以及撤离现场（V _Pt2，V _PdPt）在PdPtSe ₄单层中显着提高了与Pt（1 1 1）相当的催化活性。带中心模型应用到更好的理解在她的活动，其中，H的化学键能（ΔG的差₁）示出了以Pt /硒d / P能级的能量的近似线性关系。这里提出的策略将适用于其他二维材料。