Active electronic states in transition metal dichalcogenides are able to prompt hydrogen evolution by improving hydrogen absorption. However, the development of thermodynamically stable hexagonal 2H-MoS₂ as hydrogen evolution catalyst is likely to be shadowed by its limited active electronic state. Herein, the charge self-regulation effect mediated by tuning Mo−Mo bonds and S vacancies is revealed in metastable trigonal MoS₂ (1T'''-MoS₂) structure, which is favarable for the generation of active electronic states to boost the hydrogen evolution reaction activity. The optimal 1T'''-MoS₂ sample exhibits a low overpotential of 158 mV at 10 mA cm⁻² and a Tafel slope of 74.5 mV dec⁻¹ in acidic conditions, which are far exceeding the 2H-MoS₂ counterpart (369 mV and 137 mV dec⁻¹). Theoretical modeling indicates that the boosted performance is attributed to the formation of massive active electronic states induced by the charge self-regulation effect of Mo−Mo bonds in defective 1T'''-MoS₂ with rich S vacancies.

过渡金属二硫属化物中的活性电子态能够通过提高氢吸收来促进析氢。然而，热力学稳定的六方 2H-MoS ₂作为析氢催化剂的发展可能会因其有限的活性电子态而受到影响。在此，通过调节Mo-Mo键和S空位介导的电荷自调节效应在亚稳态三角MoS ₂ (1T'''-MoS ₂ )结构中得到揭示，这有利于产生活性电子态以增强氢进化反应活性。最佳的 1T'''-MoS _{2样品在 10 mA cm} ^-2下表现出 158 mV 的低过电位和 74.5 mV dec ^-1的 Tafel 斜率在酸性条件下，远远超过 2H-MoS ₂对应物（369 mV 和 137 mV dec ^-1）。理论模型表明，提高的性能归因于在具有丰富 S 空位的缺陷 1T'''-MoS ₂中 Mo-Mo 键的电荷自调节效应诱导大量活性电子态的形成。