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A novel heterogeneous Co(II)-Fenton-like catalyst for efficient photodegradation by visible light over extended pH

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Abstract

A novel CoII-Fenton-like heterogeneous catalyst, (H3O)2[CoII(phen)(H2O)2]2[MoVI5O15(PO4)2]·4H2O (phen=1,10-phenanthroline, C12N2H8) (1), is synthesized and utilized for photocatalytic degradation of organic dyes and antibiotic in a wide range of pH. The experimental results show that 1 acting as the Fenton-like catalyst with H2O2 exhibits remarkable activity at pH 3–9 under vis-light irradiation and is merited with excellent recyclability and reusability. A variety of analytical methods, including in-situ electron paramagnetic resonance (EPR) spectroscopy and density functional theory (DFT) calculations, are applied to study the mechanism on generation of ·OH and O2·− radicals for photocatalytic degradation. It suggests that, unlike the classical Fenton process involving the redox transformation of the central cations, the generation of ·OH and O2·− radicals is associated with the substitution of the coordinating water molecules at Co(II) by H2O2 and/or OEH−, followed by the light-driven O-O bond cleavage and dissociation The outcomes of this study are striking which overcome the obstacles in the classical FeII-Fenton process, including the slow redox transformation between Fe(II) and Fe(III) and the production of massive iron precipitates especially at elevated pH It opens up new avenues for the development of the high-performance Fenton(-like) catalysts for photocatalytic degradation over extended pH and provides new insight into the related process.

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Acknowledgements

This work was supported by the National Natural Science Foundation of China (21872105, 22072107, 21802142), the Natural Science Foundation of Fujian Province (2020J01367), the Natural Science Foundation of Longyan City (2018LYF8010) and the Science & Technology Commission of Shanghai Municipality (19DZ2271500). We are indebted to Prof. Xuxu Wang (Fuzhou University) for valuable comments and suggestions.

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Authors and Affiliations

  1. Fujian Provincial Colleges and University Engineering Research Center of Solid Waste Resource Utilization (Longyan University); College of Chemistry and Material Science, Longyan University, Longyan, 364012, China

    Wu-Hua Chen, Jin-Hua Xiong & Zhi-Biao Hu

  2. Shanghai Key Laboratory of Chemical Assessment and Sustainability, School of Chemical Science and Engineering, Tongji University, Shanghai, 200092, China

    Xue Teng & Zuofeng Chen

  3. Key Laboratory for Advanced Materials, Centre for Computational Chemistry and Research Institute of Industrial Catalysis, East China University of Science and Technology, Shanghai, 200237, China

    Haifeng Wang

  4. Department of Materials Science and Engineering, College of Materials, Xiamen University, Xiamen, 361005, China

    Jin-Xiao Mi

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  1. Wu-Hua Chen
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  2. Jin-Hua Xiong
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  3. Xue Teng
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  4. Jin-Xiao Mi
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  5. Zhi-Biao Hu
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  6. Haifeng Wang
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  7. Zuofeng Chen
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Correspondence to Wu-Hua Chen, Haifeng Wang or Zuofeng Chen.

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Chen, WH., Xiong, JH., Teng, X. et al. A novel heterogeneous Co(II)-Fenton-like catalyst for efficient photodegradation by visible light over extended pH. Sci. China Chem. 63, 1825–1836 (2020). https://doi.org/10.1007/s11426-020-9885-3

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  • DOI: https://doi.org/10.1007/s11426-020-9885-3

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