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Bridging localized electron states of pyrite-type CoS2 cocatalyst for activated solar H2 evolution

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Abstract

The development of low-cost and high-active cocatalysts is one of the most significant links for photocatalytic water splitting. Herein, a novel strategy of electron delocalization modulation for transition metal sulfides has been developed by anion hybridization. P-modified CoS2 (CoS2∣P) nanocrystals were firstly fabricated via a gas-solid reaction and coupled with CdS nanorods to construct a composite catalyst for solar H2 evolution reaction (HER). The CdS/CoS2∣P catalyst shows an HER rate of 57.8 µmol·h−1, which is 18 times that of the bare CdS, 8 times that of the CdS/CoS2, and twice that of Pt/CdS. The reduced energy barrier and suppressed reverse reaction for HER on the catalyst have been predicted and explained by density functional theory (DFT) calculation. The underlying design strategy of novel cocatalysts by electron delocalization modulation may shed light on the rational development of other advanced catalysts for energy conversion.

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Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (Nos. 51872138 and 22002060), Natural Science Foundation of Jiangsu Province (No. BK20181380), Qing Lan Project, Six Talent Peaks Project in Jiangsu Province (No. XCL-029) and Priority Academic Program Development of the Jiangsu Higher Education Institutions (PAPD). Dr. Hengming Huang gratefully acknowledges the support provided by China Scholarships Council (CSC No. 202008320109) and China Postdoctoral Science Foundation (No. 2020M681564). The authors are grateful to the Australian Microscopy & Microanalysis Research Facility at the Centre for Microscopy and Microanalysis (CMM), The University of Queensland, and the Queensland node of the Australian National Fabrication Facility. The computational resources generously provided by the High-Performance Computing Center of Nanjing Tech University are greatly appreciated.

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Authors and Affiliations

  1. Jiangsu Collaborative Innovation Center for Advanced Inorganic Function Composites, Jiangsu National Synergetic Innovation Center for Advanced Materials, State Key Laboratory of Materials-Oriented Chemical Engineering, College of Materials Science and Engineering, Nanjing Tech University, Nanjing, 211816, China

    Hengming Huang, Zhenggang Fang, Menglong Sun, Ling Zhou, Kan Hu, Jiahui Kou & Chunhua Lu

  2. Nanomaterials Centre, School of Chemical Engineering, Australian Institute for Bioengineering and Nanotechnology, The University of Queensland, Brisbane, QLD, 4072, Australia

    Hengming Huang, Zhiliang Wang, Bin Luo & Lianzhou Wang

  3. Research Institute for Electronic Science and Graduate School of Environmental Science, Hokkaido University, Hokkaido, 001-0020, Japan

    Chen Xue

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  1. Hengming Huang
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  2. Chen Xue
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  3. Zhenggang Fang
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Correspondence to Jiahui Kou, Lianzhou Wang or Chunhua Lu.

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Huang, H., Xue, C., Fang, Z. et al. Bridging localized electron states of pyrite-type CoS2 cocatalyst for activated solar H2 evolution. Nano Res. 15, 202–208 (2022). https://doi.org/10.1007/s12274-021-3457-1

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