MoS₂ is a promising candidate for hydrogen evolution reaction (HER), while its active sites are mainly distributed on the edge sites rather than the basal plane sites. Herein, a strategy to overcome the inertness of the MoS₂ basal surface and achieve high HER activity by combining single-boron catalyst and compressive strain was reported through density functional theory (DFT) computations. The ab initio molecular dynamics (AIMD) simulation on B@MoS₂ suggests high thermodynamic and kinetic stability. We found that the rather strong adsorption of hydrogen by B@MoS₂ can be alleviated by stress engineering. The optimal stress of −7% can achieve a nearly zero value of ΔG_H (~ −0.084 eV), which is close to that of the ideal Pt-SACs for HER. The novel HER activity is attributed to (i) the B-doping brings the active site to the basal plane of MoS₂ and reduces the band-gap, thereby increasing the conductivity; (ii) the compressive stress regulates the number of charge transfer between (H)-(B)-(MoS₂), weakening the adsorption energy of hydrogen on B@MoS₂. Moreover, we constructed a SiN/B@MoS₂ heterojunction, which introduces an 8.6% compressive stress for B@MoS₂ and yields an ideal ΔG_H. This work provides an effective means to achieve high intrinsic HER activity for MoS₂.

中文翻译：

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通过结合单硼催化剂和压缩应变来增强MoS 2基面的氢逸出

MoS ₂是氢释放反应（HER）的有希望的候选者，而其活性位点主要分布在边缘位点而不是基面位点。在本文中，通过密度泛函理论（DFT）计算，报道了一种通过结合单硼催化剂和压缩应变来克服MoS ₂基表面惰性并实现高HER活性的策略。B @ MoS ₂上的从头算分子动力学（AIMD）模拟表明具有高的热力学和动力学稳定性。我们发现，通过应力工程可以减轻B @ MoS ₂对氢的较强吸附。−7％的最佳应力可以使ΔG _H的值几乎为零（〜-0.084 eV），接近HER的理想Pt-SAC值。新型HER活性归因于（i）B掺杂将活性位点带到MoS ₂的基面并减小了带隙，从而提高了电导率；（ii）压应力调节（H）-（B）-（MoS ₂）之间的电荷转移数，削弱了氢在B @ MoS ₂上的吸附能。此外，我们构建了的SiN / B @的MoS ₂的异质结，其引入8.6％的压缩应力对于B @的MoS ₂，并产生一个理想的Δ ģ _ħ。这项工作为实现MoS _2的高固有HER活性提供了有效的手段。