Boosting photocatalytic dehydrogenation and simultaneous selective oxidation of benzyl alcohol to benzaldehyde over flower-like MoS2 modified Zn0.5Cd0.5S solid solution

被引:8
|
作者
Wang, Zhennan [1 ]
Lu, Dingze [1 ,2 ,3 ,4 ]
Zhou, Min [1 ]
Kondamareddy, Kiran Kumar [6 ]
Zhao, Zhenhuan [5 ]
Wang, Zheng [5 ]
Wu, Junfang [1 ]
Zhang, Boyu [1 ]
Fan, Huiqing [4 ]
Ho, Wingkei [2 ,3 ]
机构
[1] Xian Polytech Univ, Sch Sci, Xian 710048, Peoples R China
[2] Educ Univ Hong Kong, Dept Sci & Environm Studies, Hong Kong, Peoples R China
[3] Educ Univ Hong Kong, Ctr Environm & Sustainable Dev CESD, Hong Kong, Peoples R China
[4] Northwestern Polytech Univ, Sch Mat Sci & Engn, State Key Lab Solidificat Proc, Xian 710072, Peoples R China
[5] Xidian Univ, Sch Adv Mat & Nanotechnol, Xian 710126, Peoples R China
[6] Fiji Natl Univ, Coll Engn, Sch Pure Sci, Dept Phys, Lautoka, Fiji
基金
中国国家自然科学基金;
关键词
Highly efficient dehydrogenation; Synergistic selective oxidation; Benzyl alcohol; Flower-like MoS2; Zn0.5Cd0.5S nanoparticles; DFT calculations; IN-SITU SYNTHESIS; HYDROGEN-PRODUCTION; H-2; GENERATION; EVOLUTION; NANOPARTICLES; HETEROJUNCTION; FABRICATION; COMPOSITE; SYSTEM;
D O I
10.1016/j.mtphys.2023.101121
中图分类号
T [工业技术];
学科分类号
08 ;
摘要
A series of MoS2/Zn0.5Cd0.5S with varying concentrations of flower-like MoS2 is prepared based on a simple and practical method with highly efficient photocatalytic dehydrogenation and simultaneous selective oxidation of benzyl alcohol (BA) to benzaldehyde (BAD). A comparative study between the composites and their two components (pristine MoS2 and Zn0.5Cd0.5S) is carried out for various structural, optical, electrical, and photo catalytic characterization. The studies reveal that the size of Zn0.5Cd0.5S nanoparticles is in the order of 3 similar to 5 nm and is distributed uniformly over the surface of the flower-like 350 nm sized MoS2. The optical research conducted using UV-vis diffuse reflectance spectroscopy reflecting an excellent photoresponse by the MoS2/Zn0.5Cd0.5S. The photoelectrochemical tests showed that the adding of proper ratio of flower-like MoS2 (6%) results in an efficient separation and migration of photogenerated carriers for pristine Zn0.5Cd0.5S nanoparticles. The photocatalytic dehydrogenation rate of BA for the 6%-MoS2/Zn0.5Cd0.5S is the highest at 3.03 mmol g(-1) h(-1), meanwhile the yield of BAD and the selective conversion of BA to BAD are 49.3% and 100%, respectively. The essential stages of the photocatalytic dehydrogenation of BA are C-. caused by the photo-generated holes, according to the EPR spectra of the PBN-carbon centered radical (PBN-C). Besides, the mechanism for improved photocatalytic dehydrogenation and synergistic selective oxidation of BA to BAD with flower-like MoS2 modified Zn0.5Cd0.5S nanoparticles was systematically studied through gas chromatography-mass spectrometry analysis and first principle density functional theory calculations. The highly efficient dehydrogenation and synergistic selective oxidation of BA to BAD for MoS2/Zn0.5Cd0.5S are mainly attributed to the introduction of MoS2 nanoflowers that can provide abundant active sites, and formed MoS2/Zn0.5Cd0.5S heterostructures could further promote the separation of photogenerated electron-hole pairs. Moreover, the valance band position of the 6%MoS2/Zn0.5Cd0.5S is more positive, so the hole at the VB position has the stronger ability to oxidize BA. This study provides a feasible method for efficiently photocatalytic dehydrogenation synergism selective oxidation of organic substrates into valuable products.
引用
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页数:15
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