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

Li, Zhi-Jun; Fan, Xiang-Bing; Li, Xu-Bing; Li, Jia-Xin; Zhan, Fei; Tao, Ye; Zhang, Xiaoyi; Kong, Qing-Yu; Zhao, Ning-Jiu; Zhang, Jian-Ping; Ye, Chen; Gao, Yu-Ji; Wang, Xu-Zhe; Meng, Qing-Yuan; Feng, Ke; Chen, Bin; Tung, Chen-Ho; Wu, Li-Zhu

doi:10.1039/c7ta01670k

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

Journal Article · Sun Jan 01 00:00:00 EST 2017 · Journal of Materials Chemistry. A

DOI:https://doi.org/10.1039/c7ta01670k· OSTI ID:1392521

Li, Zhi-Jun; Fan, Xiang-Bing;

; Li, Jia-Xin; Zhan, Fei; Tao, Ye; Zhang, Xiaoyi; Kong, Qing-Yu; Zhao, Ning-Jiu;

; Ye, Chen; Gao, Yu-Ji; Wang, Xu-Zhe; Meng, Qing-Yuan;

; Chen, Bin; Tung, Chen-Ho;

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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Research Organization:: Argonne National Lab. (ANL), Argonne, IL (United States)

Sponsoring Organization:: Ministry of Science and Technology of the People's Republic of China; National Natural Science Foundation of China (NSFC); USDOE Office of Science - Office of Basic Energy Sciences - Scientific User Facilities Division

DOE Contract Number:: AC02-06CH11357

OSTI ID:: 1392521

Journal Information:: Journal of Materials Chemistry. A, Vol. 5, Issue 21; ISSN 2050-7488

Publisher:: Royal Society of Chemistry

Country of Publication:: United States

Language:: English

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