期刊
ACS APPLIED MATERIALS & INTERFACES
卷 13, 期 16, 页码 19406-19413出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsami.1c00139
关键词
Single-atom doping; two-dimensional materials; proximity effect; chemical vapor deposition; hydrogen reaction evolution
资金
- National Natural Science Foundation of China [51732010, 91733302, 91833302]
The development of stable and low-cost catalysts to replace Pt-based ones is challenging for hydrogen evolution reaction (HER). Incorporating single foreign Fe atoms to substitute W atoms in sandwiched two-dimensional WS2 has been proposed as a strategy to enhance catalytic reactivity for HER. The charge transfer between the doped Fe atom and neighboring S atoms on the surface activates the proximate S atoms for HER.
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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