In-Plane Heterojunctions Enable Multiphasic Two-Dimensional (2D) MoS2 Nanosheets As Efficient Photocatalysts for Hydrogen Evolution from Water Reduction

Two-dimensional (2D) single-layer MoS2 nanosheets are demonstrated as efficient photocatalysts for hydrogen evolution reaction (HER) from water reduction, thanks to specific in-plane heterojunctions constructed in the MoS2 monolayer. These functional heterojunctions are formed among the different phases of chemically exfoliated MoS2 monolayers: semiconducting 2H, metallic 1T, and quasi-metallic 1T′ phases. The proportion of the three MoS2 phases can be systematically controlled via thermal annealing of the nanosheets. Interestingly, a volcano relationship is observed between the photocatalytic HER activity and the annealing temperature with an optimum activity obtained after annealing at 60 °C. First-principles calculations were integrated with experimental studies to shed light on the role of the multiphases of MoS2 and reveal that optimum photocatalytic HER activity results from the formation of the in-plane heterojunctions between 1T′ MoS2 and 2H MoS2. Importantly, this facilitates not only balanced li...

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