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Proximity Enhanced Hydrogen Evolution Reactivity of Substitutional Doped Monolayer WS2

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journal contribution
posted on 2021-04-15, 16:33 authored by Mengke Kang, Changqing Lin, Huan Yang, Yabin Guo, Lixuan Liu, Tianyu Xue, Youwen Liu, Yongji Gong, Zhisheng Zhao, Tianyou Zhai, Kun Zhai, Anmin Nie, Yingchun Cheng, Zhongyuan Liu
The development of stable and low-cost catalysts with high reactivity to replace Pt-based ones is the central focus but challenging for hydrogen evolution reaction (HER). The incorporation of single atoms into two-dimensional (2D) supports has been demonstrated as an effective strategy because of the highly active single atomic sites and extremely large surface area of two-dimensional materials. However, the doping of single atoms is normally performed on the surface suffering from low stability, especially in acidic media. Moreover, it is experimentally challenging to produce monolayered 2D materials with atomic doping. Here, we propose a strategy to incorporate single foreign Fe atoms to substitute W atoms in sandwiched two-dimensional WS2. Because of the charge transfer between the doped Fe atom and its neighboring S atoms on the surface, the proximate S atoms become active for HER. Our theoretical prediction is later verified experimentally, showing an enhanced catalytic reactivity of Fe-doped WS2 in HER with the Volmer–Heyrovsky mechanism involved. We refer to this strategy as proximity catalysis, which is expected to be extendable to more sandwiched two-dimensional materials as substrates and transition metals as dopants.

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