Abstract
Polymerization-based wastewater treatment offers reduced oxidant demand and product recovery, yet practical application is hindered by catalyst fouling and unselective reactions due to single-site competition. Here, we report a readily synthesized and scalable ZnO/CuO catalyst featuring dual functional sites that decouple pollutant and oxidant activation. Zn sites preferentially adsorb/activate organics, whereas Cu sites predominantly activate the oxidant. This site differentiation programs two pathway regimes governed by pollutant electronic structure: electron-transfer-mediated polymerization for electron-rich substrates and radical-induced mineralization for electron-deficient substrates. Importantly, radicals generated during mineralization depolymerize the accumulated foulant layer in situ, effecting autonomous catalyst regeneration with a 2.5-fold performance recovery and reduced external regeneration demand. Process performance is validated in a 200 L self-circulating reactor, maintaining 98% removal efficiency for both pollutant classes over ten cycles. Toxicological profiling across multiple biological models, supported by metabolomics, confirmed effective detoxification of multi-pollutant wastewater, including restoration of normal metabolic function in zebrafish (e.g., lipid and glutathione metabolism). This study establishes a dual-site cooperative catalysis framework that leverages intrinsic wastewater chemistry for self-regeneration, showcasing a complete trajectory from atomic-scale design to reactor-scale implementation.
Data availability
The data supporting the findings of the study are included in the main text and supplementary information files. Raw data can be obtained from the corresponding authors upon request. Source data are provided in this paper. Source data are provided with this paper.
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Acknowledgements
The authors thank the National Natural Science Foundation of China (225B2602, 52270149), New Chongqing Youth Innovative Talent Program (CSTB2025YITP-QCRCX0056), and the Fundamental Research Funds for the Central Universities grant (2024IAIS-QN013) for supporting this work. The authors also thank Scientific Compass (www.shiyanjia. com) for supporting the related characterizations.
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F. Chen and Z.Q. Zhang conceived and planned the experiments. Z.Q. Zhang performed the relevant experiments. P.J. Duan performed the theoretical calculations. Y. Shao supervised the zebrafish experiments. Z.Q. Zhang, X.W. Xu, P.J. Duan, Z.H. Qin, Q. Wang, Y. Shao, C. W. Bai, X. J. Chen, J. Wang, F.Q. Yang, and F. Chen assisted in analyzing various characterizations. Z.Q. Zhang wrote the initial draft, X.W. Xu, P.J. Duan and F. Chen further modified the manuscript.
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Zhang, ZQ., Xu, XW., Duan, PJ. et al. Heterointerface-engineered ZnO/CuO bimetallic sites enable pollutant-directed conversion with in situ catalyst regeneration. Nat Commun (2026). https://doi.org/10.1038/s41467-026-71644-0
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DOI: https://doi.org/10.1038/s41467-026-71644-0
