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Organic wastewater treatment by a single-atom catalyst and electrolytically produced H2O2

Abstract

The presence of organic contaminants in wastewater poses considerable risks to the health of both humans and ecosystems. Although advanced oxidation processes that rely on highly reactive radicals to destroy organic contaminants are appealing treatment options, substantial energy and chemical inputs limit their practical applications. Here we demonstrate that Cu single atoms incorporated in graphitic carbon nitride can catalytically activate H2O2 to generate hydroxyl radicals at pH 7.0 without energy input, and show robust stability within a filtration device. We further design an electrolysis reactor for the on-site generation of H2O2 from air, water and renewable energy. Coupling the single-atom catalytic filter and the H2O2 electrolytic generator in tandem delivers a wastewater treatment system. These findings provide a promising path toward reducing the energy and chemical demands of advanced oxidation processes, as well as enabling their implementation in remote areas and isolated communities.

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Fig. 1: Schematic drawing of our wastewater treatment system.
Fig. 2: Characterization of Cu-C3N4.
Fig. 3: Catalytic activity and degradation product.
Fig. 4: Fenton filter.
Fig. 5: Electrodes and electrolytes of H2O2 electrolyser.
Fig. 6: Reactor design and performance of the H2O2 electrolyser.

Data availability

The data that support the findings of this study are available from the corresponding author upon request.

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Acknowledgements

Part of this work was performed at the Stanford Nano Shared Facilities, supported by the National Science Foundation under award no. ECCS-1542152. Use of the Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, was supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences under contract no. DE-AC02-76SF00515. Work at the Molecular Foundry was supported by the Office of Science, Office of Basic Energy Sciences, of the US Department of Energy under contract no. DE-AC02-05CH11231. The teratogenicity experiment was supported by NIH grant no. R35 GM127030.

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Contributions

J.X. and Y.C. conceived the idea. J.X. performed the experiments. X.Z. performed the EXAFS and STEM characterizations. Z.F. performed the teratogenicity studies. Z.L. synthesized the O-SP. W.H., Y.L. and Z.Z. performed the HR-TEM and EDS characterizations. D.V. and Y.L. helped with the HPLC and LC–MS measurements. S.D. helped with the STEM characterizations. K.W. synthesized Cu-TMCPP. Z.L. and G.C. helped with quantification of H2O2. H.W. and Z.Z. helped with electrochemistry experiments. J.X. and Y.C. wrote the manuscript with input from all co-authors.

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Correspondence to Yi Cui.

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Supplementary Information

Supplementary Figs. 1–13 and Discussion.

Supplementary Video

Filtration process of the Fenton filter.

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Xu, J., Zheng, X., Feng, Z. et al. Organic wastewater treatment by a single-atom catalyst and electrolytically produced H2O2. Nat Sustain 4, 233–241 (2021). https://doi.org/10.1038/s41893-020-00635-w

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