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Issue 21, 2017
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Direct synthesis of all-inorganic heterostructured CdSe/CdS QDs in aqueous solution for improved photocatalytic hydrogen generation

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Abstract

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 H2 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 H2 evolution.

Graphical abstract: Direct synthesis of all-inorganic heterostructured CdSe/CdS QDs in aqueous solution for improved photocatalytic hydrogen generation

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Publication details

The article was received on 23 Feb 2017, accepted on 21 Apr 2017 and first published on 24 Apr 2017


Article type: Paper
DOI: 10.1039/C7TA01670K
Citation: J. Mater. Chem. A, 2017,5, 10365-10373
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    Direct synthesis of all-inorganic heterostructured CdSe/CdS QDs in aqueous solution for improved photocatalytic hydrogen generation

    Z. Li, X. Fan, X. Li, J. Li, F. Zhan, Y. Tao, X. Zhang, Q. Kong, N. Zhao, J. Zhang, C. Ye, Y. Gao, X. Wang, Q. Meng, K. Feng, B. Chen, C. Tung and L. Wu, J. Mater. Chem. A, 2017, 5, 10365
    DOI: 10.1039/C7TA01670K

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