Journal
CHEMICAL ENGINEERING JOURNAL
Volume 431, Issue -, Pages -Publisher
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2021.134000
Keywords
Photocatalytic H-2 evolution; Lower-coordinated S atoms; Internal electric field; Interfacial chemical bond; Z-scheme-dominated; CdSe/S-L-ZnIn2S4/MoSe2
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Funding
- National Natural Sci-ence Foundation of China [52072196, 52002199, 52002200, 52102106]
- Major Basic Research Program of Natural Science Foundation of Shandong Province [ZR2020ZD09]
- Natural Science Foundation of Shandong Province [ZR2019BEM042, ZR2020QE063]
- Innovation and Technology Pro-gram of Shandong Province [2020KJA004]
- Open Project of Chemistry Department of Qingdao University of Science and Technology [QUSTHX201813]
- Taishan Scholars Program of Shandong Province [ts201511034]
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A ternary dual direct Z-scheme-dominated heterostructure was fabricated, and by optimizing its structure and interfacial chemical bond, high efficiency solar energy conversion was achieved.
Purposefully design and steering charge flow in heterostructure remains a crucial challenge for realizing efficient solar-to-fuel conversion. Herein, a newfangled ternary dual direct Z-scheme-dominated heterostructure of CdSe/ lower-coordinated S atoms (S-L)-rich ZnIn2S4/MoSe2 (CdSe/S-L-ZIS/MoSe2) is fabricated, where the lower-coordinated S atoms in ZIS can serve as the highly active sites for anchoring CdSe and MoSe2 on the surface of ZIS through Cd-S and Mo-S bonds. The optimized CdSe/S-L-ZIS/MoSe2 displays the ultrahigh visible-light (lambda > 420 nm) driven H(2)production rate of 70789.2 umol center dot g(- 1)center dot h(-1) with an apparent quantum efficiency (AQE) of 44.1% at 420 nm. Mechanism analysis and DFT calculations reveal that the interfacial chemical bond contributes to the intense internal electric field (IEF) in CdSe/S-L-ZIS/MoSe2, and finally lead to the direct Z-scheme-dominated and II-scheme-assisted charge transfer mechanism. This work establishes an atomic-scale interfacial engineering design model on directionally modulating charge transfer for efficient solar energy conversion applications.
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