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Electro-driven cycling Fenton catalysis through two-dimensional electroresponsive metal–organic frameworks for water purification

Nature Water volume 2, pages 793–802 (2024)Cite this article

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Abstract

The electro-Fenton process is a promising technology for eliminating emerging organic pollutants from water. However, its potential is hindered by the lack of cathode materials with the essential cycling catalytic functionality for sustained Fenton reactions. In this study, we developed an innovative catalytic cathode comprising a two-dimensional electroresponsive ferrocene metal–organic framework (ER-Fc-MOF) for effective H2O2 activation in a reagent-free dual-cathode electro-Fenton process. The ER-Fc-MOF cathode also enables the electro-driven regeneration of the Fe(II) sites through direct electron transfer within the ferrocene sandwich structure, achieving continuous cycling of the Fc+-Fe(III)/Fc-Fe(II) species for Fenton reactions. Electron paramagnetic resonance and quenching tests confirmed that the ER-Fc-MOF catalytic cathode generates both radical (HO·) and non-radical (1O2) species for highly efficient degradation of organic pollutants across a broad pH range in diverse water matrices. This novel electroresponsive cycling catalyst for the electro-Fenton process presents a promising route towards the development of green and sustainable oxidation technologies for water purification and wastewater treatment.

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Fig. 1: Schematic of the novel dual-cathode electro-Fenton system.
Fig. 2: Characterization of the ER-Fc-MOF cathode material.
Fig. 3: Catalytic performance of ER-Fc-MOF, FeNi-MOF and NiF as cathode materials in the electro-Fenton process.
Fig. 4: Determination of reactive species and the proposed mechanism for electroresponsive catalysis in the electro-Fenton system.
Fig. 5: Catalytic performance of the ER-Fc-MOF cathode for SMX removal from wastewater.

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Data availability

The data supporting the findings of this study are available within the paper and its Supplementary Information. Source data are provided with this paper.

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Acknowledgements

This research was financially supported by the National Natural Science Foundation of China (project nos 52100093 for L.L. and 52270128 for X.-y.L.), the Basic and Applied Basic Research Foundation of the GuangDong Government (project nos 2021B1515120068 for X.-y.L. and 2023A1515011734 for L.L.), the Municipal Science and Technology Innovation Commission of the Shenzhen Government (project nos KCXFZ20211020163556020 and SGDX20230116092359002 for L.L.), the Research Grants Council (project nos 17210219 for X.-y.L.) and the Innovation and Technology Fund (project no. ITS/242/20FP for X.-y.L.) of the Hong Kong Government, China.

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Authors and Affiliations

  1. School of Environmental Science and Engineering, Sun Yat-sen University, Guangzhou, China

    Chao Yang & Lianpeng Sun

  2. Environmental Engineering Research Centre, Department of Civil Engineering, The University of Hong Kong, Hong Kong, China

    Chao Yang, Pei Wang, Zhihong Ye, Yixuan Wang, Kaimin Shih & Xiao-yan Li

  3. School of Environment and Energy, South China University of Technology, Guangzhou, China

    Shanshan Shang

  4. Institute of Environment and Ecology, Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen, China

    Lin Lin & Xiao-yan Li

  5. Key Laboratory of Eco-environments in Three Gorges Reservoir Region, Ministry of Education, College of Environment and Ecology, Chongqing University, Chongqing, China

    Zhihong Ye

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Contributions

C.Y. and X.-y.L. led the project and designed the study; C.Y. and S.S. performed the experiments with the assistance of P.W. and Y.W.; C.Y., S.S., L.L., Z.Y., K.S., L.S. and X.-y.L. contributed to the interpretation of the data; C.Y., S.S., L.L. and X.-y.L. co-wrote the paper.

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Correspondence to Shanshan Shang, Lin Lin or Xiao-yan Li.

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Yang, C., Shang, S., Lin, L. et al. Electro-driven cycling Fenton catalysis through two-dimensional electroresponsive metal–organic frameworks for water purification. Nat Water 2, 793–802 (2024). https://doi.org/10.1038/s44221-024-00262-1

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