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An Integrated Photoelectrochemical–Chemical Loop for Solar-Driven Overall Splitting of Hydrogen Sulfide

Authors

  • Dr. Xu Zong,

    1. Nanomaterials Centre, School of Chemical Engineering and Australian Institute for Bioengineering and Nanotechnology, The University of Queensland, QLD 4072 (Australia)
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  • Jingfeng Han,

    1. State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences and Dalian Laboratory for Clean Energy, Dalian 116023 (China) http://www.canli.dicp.ac.cn
    2. Graduate University of Chinese Academy of Sciences, Beijing 100049 (China)
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  • Dr. Brian Seger,

    1. Department of Physics, CINF, Technical University of Denmark, 2800 Kongens Lyngby (Denmark)
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  • Dr. Hongjun Chen,

    1. Nanomaterials Centre, School of Chemical Engineering and Australian Institute for Bioengineering and Nanotechnology, The University of Queensland, QLD 4072 (Australia)
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  • Prof. Gaoqing (Max) Lu,

    1. Nanomaterials Centre, School of Chemical Engineering and Australian Institute for Bioengineering and Nanotechnology, The University of Queensland, QLD 4072 (Australia)
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  • Prof. Dr. Can Li,

    Corresponding author
    1. State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences and Dalian Laboratory for Clean Energy, Dalian 116023 (China) http://www.canli.dicp.ac.cn
    • Can Li, State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences and Dalian Laboratory for Clean Energy, Dalian 116023 (China) http://www.canli.dicp.ac.cn

      Lianzhou Wang, Nanomaterials Centre, School of Chemical Engineering and Australian Institute for Bioengineering and Nanotechnology, The University of Queensland, QLD 4072 (Australia)

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  • Prof. Lianzhou Wang

    Corresponding author
    1. Nanomaterials Centre, School of Chemical Engineering and Australian Institute for Bioengineering and Nanotechnology, The University of Queensland, QLD 4072 (Australia)
    • Can Li, State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences and Dalian Laboratory for Clean Energy, Dalian 116023 (China) http://www.canli.dicp.ac.cn

      Lianzhou Wang, Nanomaterials Centre, School of Chemical Engineering and Australian Institute for Bioengineering and Nanotechnology, The University of Queensland, QLD 4072 (Australia)

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  • This project was supported by the Australian Research Council (through its DP and FT programs) and Queensland State Government Smart State program (NIRAP). This work was performed in part at the Qld node of the Australian National Fabrication Facility. We gratefully acknowledge the Danish Ministry of Science for funding the Catalysis for Sustainable Energy (CASE) initiative and the Danish National Research Foundation for founding The Center for Individual Nanoparticle Functionality. We also thank Thomas Pedersen (DTU) for providing p-n junction Si wafers.

Abstract

Abundant and toxic hydrogen sulfide (H2S) from industry and nature has been traditionally considered a liability. However, it represents a potential resource if valuable H2 and elemental sulfur can be simultaneously extracted through a H2S splitting reaction. Herein a photochemical-chemical loop linked by redox couples such as Fe2+/Fe3+ and I/I3 for photoelectrochemical H2 production and H2S chemical absorption redox reactions are reported. Using functionalized Si as photoelectrodes, H2S was successfully split into elemental sulfur and H2 with high stability and selectivity under simulated solar light. This new conceptual design will not only provide a possible route for using solar energy to convert H2S into valuable resources, but also sheds light on some challenging photochemical reactions such as CH4 activation and CO2 reduction.

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