Journal
APPLIED CATALYSIS B-ENVIRONMENTAL
Volume 298, Issue -, Pages -Publisher
ELSEVIER
DOI: 10.1016/j.apcatb.2021.120534
Keywords
Photoredox; Perylenetetracarboxylic diimide; Graphitic carbon nitride; Z-scheme heterojunction; Metal-free photocatalyst
Funding
- National Natural Science Foundation of China [91233108, 21703287]
- Natural Science Foundation of Shandong Province [ZR2017MB006, ZR2017BB027, ZR2020QB057]
- Major Program of Shandong Province Natural Science Foundation [ZR2017ZB0315]
- Fundamental Research Funds for the Central Universities [18CX02052A, 19CX05002A]
- Taishan Scholar Program of Shandong Province [ts201712019]
- China Postdoctoral Science Foundation [2020M672162]
- Talent Introduction Program of China University of Petroleum (East China) [yj20190039]
- Independent Innovation Project of China University of Petroleum (East China) [20CX06035A]
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The paper presents a robust covalently-bonded direct Z-scheme heterostructure (PDI/mpgCN) for the photocatalytic oxidative coupling of amines, which shows remarkable enhancement in amine oxidation rate compared to pristine g-C3N4. The study provides insight into heterojunction design with chemical bond precision and highlights the great prospects of Z-scheme photocatalyst in photo-chemical synthesis.
Photocatalytic oxidative coupling of amines is a promising method for imine synthesis. In this paper, a robust covalently-bonded direct Z-scheme heterostructure (PDI/mpgCN) for photocatalytic oxidative coupling of amine was reported for the first time. Perylenetetracarboxylic diimide (PDI) molecules were covalently connected to the surface of mesoporous carbon nitride (mpgCN) via an in-situ condensation strategy. Compared with the poor conversion efficiency upon pristine g-C3N4, PDI/mpgCN heterostructure exhibits a remarkable enhancement on amine oxidation rate (AOR), with the optimal AOR reaches to as high as 20.63 mmol g(-1) h(-1) upon 20 % PDI/mpgCN. As far as we know, it is the highest AOR achieved so far for amine photooxidation coupling with heterojunction materials. Transient absorption studies proved the formation of Z-scheme junction, and efficient interfacial charge transfer. Our study not only makes an insight into the heterojunction design with chemical bond precision, but highlights the great prospects of Z-scheme photocatalyst in photo-chemical synthesis.
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