Journal
CHEMICAL ENGINEERING JOURNAL
Volume 430, Issue -, Pages -Publisher
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2021.133125
Keywords
Photocatalytic hydrogen production; Oxidative dehydrogenation; S-scheme heterojunction; Defect and doping engineering; Charge separation
Categories
Funding
- National Natural Science Foundation of China [21908187, 22169021]
- Project of Science & Technology Office of Shaanxi Province [2021KJXX-41, 2021JQ-611]
- Special projects for high-level talents of Yan'an city [2019-02]
- Startup Foundation for Docotors of Yan'an University [YDBK2018-41, YDBK2018-42]
- Research Program of Yan'an University [YDY2019-23, YDY2019-21]
- Graduate Education Innovation Project of Yan'an University [YCX2020002]
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A well-designed S-scheme O-ZnIn2S4/TiO2-x heterojunction was fabricated to achieve efficient photocatalytic hydrogen production via water reduction coupled with organic oxidative dehydrogenation. The synergistic effect of oxygen defect and doping engineering led to improved charge transfer and separation efficiency at the interface, resulting in remarkable H-2 and benzaldehyde production rates. The coupled reaction system displayed superior H-2 evolution activity compared to sacrificial reagent systems, with both water and organic molecules providing protons for H-2 production.
Aiming to the unwanted photocatalytic hydrogen production systems using sacrifice agents, a well-design S-scheme O-ZnIn2S4/TiO2-x heterojunction was fabricated to realize photocatalytic hydrogen production via water reduction coupled with organic oxidative dehydrogenation. As supported by DFT calculations and experimental analysis, owing to the synergistic effect of oxygen defect and doping engineering, a tailored energy band structure alignment with higher redox potentials and larger Fermi level potential difference are achieved, resulting in more efficient S-scheme interface charge transfer and separation efficiency, thus improving the photocatalytic activity of O-ZnIn2S4/TiO2-x. The optimal O-ZnIn2S4/TiO2-x photocatalyst shows remarkable H-2 and benzaldehyde production rate of 2584.9 mu mol g(-1)h(-1) and 2880.5 mu mol g(-1)h(-1) under visible light, which are 52.5 and 66.4 times as high as those over blank TiO2. Interestingly, this coupled reaction system also displays superior H-2 evolution activity compared to sacrificial reagent systems of Na2SO3/Na2S and triethanolamine. Further quenching and EPR experiments reveal that both water and organic molecules provide protons for H-2 production.
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