Journal
JOURNAL OF MATERIALS CHEMISTRY A
Volume 5, Issue 21, Pages 10365-10373Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c7ta01670k
Keywords
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Funding
- Ministry of Science and Technology of China [2013CB834505, 2014CB239402, 2013CB834804]
- National Science Foundation of China [91427303, 21390404, 21403260, U1332205, 51373193]
- Chinese Academy of Science [XDB17030300]
- Youth Innovation Promotion Association of Chinese Academy of Sciences [2016022]
- DOE Office of Science [DE-AC02-06CH11357]
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Here we present a facile aqueous approach to synthesize heterostructured CdSe/CdS QDs with all-inorganic chalcogenide S2- ligands under mild conditions. High-resolution transmission electron microscopy (HRTEM), X-ray diffraction (XRD), Raman spectroscopy, X-ray photoelectron spectroscopy (XPS), and steady-state emission spectroscopy demonstrate that the heterostructured CdSe/CdS QDs with sulfur-rich surface composition are formed by heterogeneous nucleation of Cd2+ and S2- precursors on the CdSe QDs. After adsorption of small Ni(OH)(2) clusters over the surface in situ, the CdSe/CdS-Ni(OH)(2) photocatalyst enables H-2 production efficiently with an internal quantum yield of 52% under visible light irradiation at 455 nm, up to an 8-fold increase of activity to that of spherical CdSe QDs-Ni(OH)(2) under the same conditions. Femtosecond transient absorption spectroscopy, X-ray transient absorption (XTA) spectroscopy, steady-state and time-resolved emission spectroscopy show that the quasi-type-II band alignment in the CdSe/CdS heterostructure is responsible for the efficiency enhancement of light harvesting and surface/interfacial charge separation in solar energy conversion. The unprecedented results exemplify an easily accessible pattern of aqueous synthesis of all-inorganic heterostructured QDs for advanced photosynthetic H-2 evolution.
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