Journal
CHEMSUSCHEM
Volume 7, Issue 5, Pages 1468-1475Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cssc.201400028
Keywords
biomass; hydrogen production; photocatalysis; quantum dots; water splitting
Funding
- Ministry of Science and Technology of China [2014CB239402, 2013CB834804, 2013CB834505]
- National Science Foundation of China [2109343, 21390404, 91027041, 51373193]
- Solar Energy Initiative of the Knowledge Innovation Program of the Chinese Academy of Sciences
- Bureau for Basic Research of the Chinese Academy of Sciences
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Natural photosynthesis offers the concept of storing sunlight in chemical form as hydrogen (H-2), using biomass and water. Herein we describe a robust artificial photocatalyst, nickel-hybrid CdS quantum dots (Ni-h-CdS QDs) made insitu from nickel salts and CdS QDs stabilized by 3-mercaptopropionic acid, for visible-light-driven H-2 evolution from glycerol and water. With visible light irradiation for 20h, 403.2mol of H-2 was obtained with a high H-2 evolution rate of approximately 74.6molh(-1)mg(-1) and a high turnover number of 38405 compared to MPA-CdS QDs (mercaptopropionic-acid-stabilized CdS quantum dots). Compared to CdTe QDs and CdSe QDs, the modified CdS QDs show the greatest affinity toward Ni2+ ions and the highest activity for H-2 evolution. X-ray photoelectron spectroscopy (XPS), inductively-coupled plasma atomic emission spectrometry (ICP-AES), and photophysical studies reveal the chemical nature of the Ni-h-CdS QDs. Electron paramagnetic resonance (EPR) and terephthalate fluorescence measurements clearly demonstrate water splitting to generate OH radicals. The detection of DMPO-H and DMPO-C radicals adduct in EPR also indicate that H radicals and C radicals are the active species in the catalytic cycle.
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