Journal
JOURNAL OF CATALYSIS
Volume 281, Issue 2, Pages 318-324Publisher
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcat.2011.05.015
Keywords
Photocatalysis; Hydrogen; Hybrid system; Semiconductor; Cobaloximes catalysts
Categories
Funding
- National Basic Research Program of China [2009CB220010]
- National Natural Science Foundation of China (NSFC) [21090341, 21061140361]
- Programme Strategic Scientific Alliances China and the Netherlands [2008DFB50130]
- Chinese Academy of Sciences [KGCX2-YW-391]
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An artificial photocatalytic system mimicking photosystem I (PSI) has been assembled using semiconductor (CdS) as photosensitizer, cobaloximes (Co-III complexes) as H-2 evolution catalysts, and triethanolamine (TEOA) as sacrificial electron donor. This artificial photocatalytic system shows high hydrogen evolution activity (turnover number up to 171 based on Co-III(dmgH)(2)pyCl 1) under visible light irradiation. The apparent quantum efficiency (QE) for 1/CdS hybrid photocatalytic system in acetonitrile solution at 420 nm is calculated to be 9.1%. The interfacial electron transfer from photoexcited CdS to Co-III complexes is very efficient through the weak adsorption of Co-III complexes on CdS. The adsorption of 1 on CdS in acetonitrile fits Langmuir equation, the maximum monolayer adsorption capacity is 3 x 10(-3) mmol g(-1), which means most of 1 are in the solution. The rate of hydrogen production exhibits a quadratic dependence on the total concentration of I. Therefore, a bimetallic catalysis pathway is proposed. The efficient electron transfer, the broad electronic absorption character of CdS photosensitizer as well as the H-2 evolution ability of Co-III complexes, account for the high photocatalytic activity of this hybrid photocatalytic system. (C) 2011 Elsevier Inc. All rights reserved.
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