Journal
CHEMICAL ENGINEERING JOURNAL
Volume 429, Issue -, Pages -Publisher
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2021.132229
Keywords
Vanadium single atom; Carbon nitride; Photocatalysis; Hydrogen evolution; Formaldehyde oxidation
Categories
Funding
- National Natural Science Foundation of China [52104254, 51472194, 21975193]
- Science and Tech-nology Planning Project of Shenzhen Municipality [JCYJ20200109150225155]
- Research Project of Hubei Provincial Department of Education [Q20202501]
- Hubei Key Laboratory of Pollutant Analysis & Reuse Technology Open Foundation [PA200208]
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By designing coordinating single-atomic-site V on ultrathin carbon nitride with V-N charge-transfer bridge, high efficient photocatalytic H2 production and formaldehyde oxidation under visible light were achieved. This design significantly improves photocatalytic efficiency and outperforms other carbon nitride-based photocatalysts.
Solar-driven hydrogen evolution and formaldehyde oxidation are highly appealing, but insufficient active sites and restricted charge transfer channel resulted in limited photocatalytic efficiency for most reaction systems. Herein, we designed coordinating single-atomic-site V on ultrathin carbon nitride (namely, SAVCN) with V-N charge-transfer bridge as the reaction switch for photocatalytic H2 production and formaldehyde oxidation under visible light. The formation of V single-atoms was certified by spherical aberration-corrected HAADF-STEM, EXAFS, and DFT study. The electronic structure of the V-N bridge enables a stable photocatalytic hydrogen evolution activity, which is nearly 3 times above that of pristine carbon nitride under 420 nm, and further elevates the green light driven H2 generation by over 11-fold. Remarkably, the SAVCN system exhibits comparably high photocatalytic activity for gaseous formaldehyde oxidation, which is superior to most reported carbon nitride-based photocatalysts. The photocatalytic mechanistic prediction confirms that the introduced unsaturated V-N coordination favorably reduces the activation energy barrier of the hydrogen evolution, and enhances the rate-determining step of intermediates for mineralization of gaseous formaldehyde.
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