Journal
APPLIED CATALYSIS B-ENVIRONMENTAL
Volume 199, Issue -, Pages 134-141Publisher
ELSEVIER
DOI: 10.1016/j.apcatb.2016.06.029
Keywords
Artificial photosynthesis; Cobaloxime coenzyme; Hydrogen generation
Funding
- National Natural Science Foundation of China [51323011, 51236007]
- Program for New Century Excellent Talents in University [NCET-13-0455]
- Natural Science Foundation of Shaanxi Province [2014KW07-02]
- Natural Science Foundation of Jiangsu Province [BK 20141212]
- Nano Research Program of Suzhou City [ZXG201442, ZXG 2013003]
- Foundation for the Author of National Excellent Doctoral Dissertation of P. R. China [201335]
- National Program for Support of Top-notch Young Professionals
- Fundamental Research Funds for the Central Universities
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Inspired by the natural photosynthesis, artificial photosynthesis (AP) systems comprised of light harvesters and redox catalysts have been widely investigated for photocatalytic I:12 generation. Here we report an artificial photosynthesis system composed of CdS nanocrystals as photosensitizer, cobaloxime coenzyme (Co(dmgBF(2))(2)(H2O)(2), Co) as catalyst, and lactic acid (LA) as electron donor for H-2 generation in a fully aqueous solution. This CdS/Co/LA system exhibits exceptional high photocatalytic activity under visible light, with initial H-2 generation rate increased by 4000% compared to CdS/LA, which is even 700% as high as that of CdS/Pt/LA. The excellent photocatalytic performance of CdS/Co/LA should be attributed to the efficient electron transfer from CdS to Co, leading to the reduced charge recombination, as well as the, positively shifted Fermi level of CdS, decreasing the overpotential for H-2 generation. Moreover, the electron-coupling-electron-coupling (ECEC) mechanism, involving with the reduction of Co coenzyme followed by protonation and then reduction again, was supposed to produce the Co(II)-H intermediate active for catalyzing. H-2 evolution from aqueous solution. (C) 2016 Elsevier B.V. All rights reserved.
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