Photocatalytic Hydrogen Evolution from Glycerol and Water over Nickel-Hybrid Cadmium Sulfide Quantum Dots under Visible-Light Irradiation

Authors

  • Jiu-Ju Wang,

    1. Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry & University of Chinese Academy of Sciences, The Chinese Academy of Sciences, Beijing, 100190 (PR China), Fax: (+86) 10-8254-3580
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    • These authors contributed equally to this work.

  • Dr. Zhi-Jun Li,

    1. Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry & University of Chinese Academy of Sciences, The Chinese Academy of Sciences, Beijing, 100190 (PR China), Fax: (+86) 10-8254-3580
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    • These authors contributed equally to this work.

  • Xu-Bing Li,

    1. Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry & University of Chinese Academy of Sciences, The Chinese Academy of Sciences, Beijing, 100190 (PR China), Fax: (+86) 10-8254-3580
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  • Xiang-Bing Fan,

    1. Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry & University of Chinese Academy of Sciences, The Chinese Academy of Sciences, Beijing, 100190 (PR China), Fax: (+86) 10-8254-3580
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  • Dr. Qing-Yuan Meng,

    1. Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry & University of Chinese Academy of Sciences, The Chinese Academy of Sciences, Beijing, 100190 (PR China), Fax: (+86) 10-8254-3580
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  • Shan Yu,

    1. Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry & University of Chinese Academy of Sciences, The Chinese Academy of Sciences, Beijing, 100190 (PR China), Fax: (+86) 10-8254-3580
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  • Cheng-Bo Li,

    1. Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry & University of Chinese Academy of Sciences, The Chinese Academy of Sciences, Beijing, 100190 (PR China), Fax: (+86) 10-8254-3580
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  • Jia-Xin Li,

    1. Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry & University of Chinese Academy of Sciences, The Chinese Academy of Sciences, Beijing, 100190 (PR China), Fax: (+86) 10-8254-3580
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  • Prof. Dr. Chen-Ho Tung,

    1. Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry & University of Chinese Academy of Sciences, The Chinese Academy of Sciences, Beijing, 100190 (PR China), Fax: (+86) 10-8254-3580
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  • Prof. Dr. Li-Zhu Wu

    Corresponding author
    1. Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry & University of Chinese Academy of Sciences, The Chinese Academy of Sciences, Beijing, 100190 (PR China), Fax: (+86) 10-8254-3580
    • Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry & University of Chinese Academy of Sciences, The Chinese Academy of Sciences, Beijing, 100190 (PR China), Fax: (+86) 10-8254-3580

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Abstract

Natural photosynthesis offers the concept of storing sunlight in chemical form as hydrogen (H2), using biomass and water. Herein we describe a robust artificial photocatalyst, nickel-hybrid CdS quantum dots (Nih-CdS QDs) made in situ from nickel salts and CdS QDs stabilized by 3-mercaptopropionic acid, for visible-light-driven H2 evolution from glycerol and water. With visible light irradiation for 20 h, 403.2 μmol of H2 was obtained with a high H2 evolution rate of approximately 74.6 μmol h−1 mg−1 and a high turnover number of 38 405 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 H2 evolution. X-ray photoelectron spectroscopy (XPS), inductively-coupled plasma atomic emission spectrometry (ICP-AES), and photophysical studies reveal the chemical nature of the Nih-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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