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

MoS 2 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 MoS 2 -based electrocatalysts. To address this issue, we have developed an in situ sulfurization strategy for constructing bent MoS 2 nanosheet-coated amorphous MoO x composites (B-MoS 2 @MoO x -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 MoS 2 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 MoS 2 layers and increasing the interlayer binding energy. With these benefits, the overpotential that requires for B-MoS 2 @MoO x -C to achieve a current density of 1.0 A cm –2 in 0.5 M H 2 SO 4 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.