期刊
APPLIED CATALYSIS B-ENVIRONMENTAL
卷 294, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.apcatb.2021.120259
关键词
Carbon nitride; Donor-acceptor; Photocatalysis; Organic synthesis; Oxidization
资金
- National Natural Science Foundation of China [21961142019, 22072020, 22032002, U1905214, 21861130353, 21761132002, 21425309]
- National Key R&D Program of China [2018YFA0209301]
- Science Foundation of the Fujian Province [2019J01203]
- Chang Jiang Scholars Program of China [T2016147]
- 111 Project [D16008]
- outstanding youth scientific research personnel training plan of colleges and universities in Fujian Province
Selective oxidation reactions play a key role in converting petrochemical feedstock into commodity chemicals and pharmaceuticals, but efficiency and selectivity are often limited. A donor-acceptor functional carbon nitride photocatalyst (ECN) was developed through surface engineering photochemical modification, showing significant enhancement in the photocatalytic aerobic oxidation of alcohols under 620 nm red-light irradiation.
Oxidation, especially selective oxidation by a heterogeneous catalyst with molecular oxygen, is a core technology for the conversion of petrochemical feedstock to commodity chemicals and pharmaceuticals. Existing catalytic approaches for efficient aerobic oxidation normally rely on the engagement of organometallic centers or transition-metal nanoparticles. In light of the necessity to develop sustainable production methodologies, multiple approaches for the metal-free polymeric carbon nitride (PCN) photocatalytic selective oxidation have been evaluated. However, the insufficient visible light optical absorption, poor charge-carriers separation and the weak driving force towards oxidation reaction impart a serious restriction on the efficiency and selectivity of the organic photosynthesis, especially under extended wavelength solar light irradiation. Here, we report a surface engineering photochemical modification method to fabricate a donor-acceptor (D-A) functional carbon nitride photocatalyst (ECN) under ambient conditions. The well-developed D-A structure, preserved high crystallinity and enlarged pi-conjugation framework of the hybrid semiconductor-molecule ECN samples favor the improvement of the optical absorption, as well as the enhanced separation and migration of the photo-generated charge carriers. As a result, the obtained ECN photocatalysts exhibited remarkable enhancement in the photocatalytic aerobic oxidation of alcohols, even under an extended light wavelength of 620 nm red-light irradiation. The photocatalytic aerobic sulfides and sp3 C-H oxidation reactions were also considerably accelerated over ECN and may serve as a direct approach for the construction of value-added sulfoxide and ketone products.
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