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Heterostructure Induced S p‐Band Center Shift for Activating 1T‐MoS2 Basal Plane towards Hydrogen Evolution Reaction

Von Wiley-VCH zur Verfügung gestellt

We constructed abundant hetero-interfaces by electrodepositing CoS2 nanoparticles on the 1T-MoS2 basal plane. The hetero-interface S atoms reveal up-shifted p-band centers relative to those S atoms in the basal plane, which optimizes the ΔGH* and activates the 1T-MoS2 basal plane with enhanced hydrogen evolution activity. The electrocatalyst demonstrated excellent HER activity and robust stability.


Abstract

Despite the benefits of metallic conductivity and highly active edge Mo sites of 1T phase molybdenum disulfide (1T-MoS2) as an electrocatalyst, its overall catalytic efficiency for hydrogen evolution reaction (HER) is still limited by the less active S sites on the basal plane with a considerable positive ΔGH*. As a result, activating the basal plane S atoms is a viable solution for increasing catalytic activity. In this work, we modulated the electronic structure of 1T-MoS2 by constructing a heterostructure with CoS2 nanoparticles deposited on the 1T-MoS2 basal plane. This heterostructure demonstrated excellent HER activity as well as robust stability. Theoretical calculations indicate that the bridge S atoms connecting 1T-MoS2 and CoS2 have an up-shifted p-band center relative to the S atoms on the basal plane, so the ΔGH* of the bridge S atoms is optimized to thermal neutrality and the 1T-MoS2 basal plane is activated with enhanced hydrogen evolution activity. This work provides a novel strategy for activating the basal plane S atoms of 1T-MoS2.

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