Sulfur vacancies-induced “Electron Bridge” in Ni4Mo/Sv-Zn Cd1-S regulates electron transfer for efficient H2-releasing photocatalysis
Journal of Energy Chemistry(2023)
摘要
Despite the existence of plentiful photocatalyst heterojunctions, their separation efficiency and charge flow precision remain low on account of lacking interfacial modulation. Herein, through a defect-induced heterojunction constructing strategy, Ni4Mo alloys were in-situ grown on the unsaturated coordinated sulfur atoms of sulfur vacancies-rich ZCS (Sv-ZCS) via interfacial Ni-S covalent bonds. The experimental and theoretical results reveal that these unsaturated sulfur atoms induced by sulfur vacancies vastly facilitate to anchor more Ni-Mo nanoparticles and form abundant Ni-S covalent bonds, meanwhile, these sulfur vacancies could form dual internal electric field (IEF) and work with Ni-S covalent bonds as “Electron Bridge” to further accelerate photoelectrons transfer, as well as promote the activation of water molecules and the desorption of hydrogen proton. Accordingly, the optimized Ni4Mo/Sv-ZCS composite achieves an improved photocatalytic hydrogen evolution (PHE) rate of 94.69 mmol h−1 g−1 without an evident decrease after 6 cycles of photocatalytic tests, which is 21.2 and 1.94 times higher than those of Pt/ZCS and Ni4Mo/ZCS, respectively. This tactic opens a new way for optimizing ZnxCd1-xS-based heterojunctions by constructing sulfur vacancies and covalent bonds as “Electron Bridge” to enhance the activity of PHE.
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关键词
photocatalysis,electron bridge”,electron transfer,sulfur,vacancies-induced
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