biostudies-literatureGuo XNational Natural Science Foundation of China (National Science Foundation of China)5954https://www.ebi.ac.uk/biostudies/studies/S-EPMC9550810biostudies-literatureUnknown13(1)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 Nature communicationsCharge self-regulation in 1T'''-MoS₂ structure with rich S vacancies for enhanced hydrogen evolution activity.PMC955081021871008, 21801247, 21872166, 21973107 and 51702345Fang YHuang FLiu JGuo XLei YZhao WXu SSong EfalseCharge self-regulation in 1T'''-MoS₂ structure with rich S vacancies for enhanced hydrogen evolution activity.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 2022-01-01T00:00:00Z2022 Oct2025-04-05T12:17:56.868Z2025-04-05T12:17:56.868ZS-EPMC95508103621695410.1038/s41467-022-33636-8