期刊
CHINESE JOURNAL OF CATALYSIS
卷 43, 期 7, 页码 1894-1905出版社
ELSEVIER
DOI: 10.1016/S1872-2067(21)64026-3
关键词
Photocatalysis; Nb2O5; Highly disordered NbO6 units; Charge-transfer process; N-hydroxyphthalimide
资金
- National Natural Science Foundation of China [22025206, 21961130378, 21802137]
- Dalian Science and Technolo-gy Innovation Fund [2019J11CY009]
- Liaoning Revitalization Talents Program [XLYC2002012]
- Dalian Innovation Support Plan for High Level Talents [2020RT10]
- Youth Innovation Promotion Association (YIPA) of the Chinese Academy of Sciences [2019185]
- Newton Advanced Fellowships [NAF\R1\191267]
This study investigates the role of different NbOx units in Nb2O5 catalysts in the activation of C-H bond under visible light irradiation using N-hydroxyphthalimide (NHPI) as a probe molecule. The results demonstrate that Nb2O5 catalysts with highly disordered NbO6 units exhibit higher activity compared to those with slightly disordered NbO6 units.
Although different NbOx units are present in Nb2O5-based catalysts, the correlations between these structures and activity remain unclear, which considerably hinders the further development of Nb2O5 photocatalysis. Herein, we utilized N-hydroxyphthalimide (NHPI) as the probe molecule to distinguish the role of different NbOx units in the activation of C-H bond under visible light irradiation. With the addition of NHPI, Nb2O5 catalysts with highly disordered NbO6 units exhibited higher activities than that with slightly disordered NbO6 units (419-495 vs. 82 mu mol.g(-1).h(-1)) in photocatalytic selective oxidation of ethylbenzene. Revealed by Raman spectra, electron paramagnetic resonance spectra, and transmission-electron-microscopy images, highly disordered NbO6 units were confirmed to act as the active sites for the transfer of photogenerated electrons from NHPI, promoting the generation of phthalimide-N-oxyl (PINO) radicals for the enhanced conversion of ethylbenzene under visible light irradiation. This study provides guidance on the role of local NbOx units in Nb2O5 photocatalysis. (C) 2022, Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. All rights reserved.
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