Engineering Bent MoS ₂ Nanosheets Promotes Stable Electrocatalytic Hydrogen Evolution at 1.0 A cm ^–2

MoS2 has been identified as a promising candidate electrocatalyst for replacing precious metals in the field of producing hydrogen. Nevertheless, the vulnerability to rapid deactivation at elevated current densities significantly restricts the industrial application of MoS2-based electrocatalysts. To address this issue, we have developed an in situ sulfurization strategy for constructing bent MoS2 nanosheet-coated amorphous MoOx composites (B-MoS2@MoOx-C) as a highly efficient electrocatalyst. Here, bending engineering causes an increase in electron occupancy in the bonding orbital and a decrease in antibonding orbital electrons on the bottom basal plane of the bent MoS2 outer layer, where the active sites are positioned, significantly enhancing the Mo–S bond energy. Additionally, our strategy effectively induces charge transfer from the S atoms on the bottom basal plane to those on the top basal plane, consequently attenuating the electrostatic repulsive force between the MoS2 layers and increasing the interlayer binding energy. With these benefits, the overpotential that requires for B-MoS2@MoOx-C to achieve a current density of 1.0 A cm–2 in 0.5 M H2SO4 is a mere 340.0 mV or so, and it can operate stably for 393 h, significantly outperforming the majority of previously reported transition metal-based electrocatalysts. Consequently, our work holds significant scientific implications for the advancement of the industrial application of such electrocatalysts.