期刊
APPLIED CATALYSIS B-ENVIRONMENTAL
卷 262, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.apcatb.2019.118144
关键词
Photocatalytic CO2 reduction; Heterostructure; Cocatalyst; Conductive MOF; Thin films
资金
- Natural Science Foundation of China [21701118]
- Natural Science Foundation of Jiangsu Province [BK20161209, BK20160323]
- Natural Science Research Project of Jiangsu Higher Education Institutions [18KJA480004]
- Key Technology Initiative of Suzhou Municipal Science and Technology Bureau [SYG201748]
- Priority Academic Program Development (PAPD) of Jiangsu Higher Education Institutions
- Soochow University-Western University Centre for Synchrotron Radiation Research
In this work, composite thin films comprising the 2D/2D MOF/rGO heterostructures assembled via Coulomb interaction are employed as the cocatalyst for photocatalytic CO2 reduction for the first time. The electrostatic charge transfer and the strong pi-pi interaction induced in the heterostructure effectively modulate the electronic structure of the metal centers in the conductive 2D MOF (Ni3HITP2), evidenced by Zeta Potentials, HR-TEM, XPS and XANES. The best thin-film catalyst with an optimal MOF/rGO ratio demonstrates a high CO evolution rate of 3.8 x 10(4) mu mol h(-1) g(film)(-1) (0.46 min(-1) in TOF) and a good selectivity of 91.74%, synergically contributed by the improved photoelectron harvesting on the rGO scaffold, the efficient charge transportation/transfer within the conductive and intimate 2D heterostructure, the coherent energy flow owing to aligned energy levels, and the enriched electron density at the isolated Ni-N-4 sites boosted by electrostatic charge transfer.
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