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Synergetic physical damage and chemical oxidation for highly efficient and residue-free water disinfection

Nature Water volume 2, pages 1226–1237 (2024) Cite this article

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Abstract

Waterborne pathogens, in particular, emerging antibiotic-resistant bacteria (ARB), can cause serious infectious diseases, posing a huge threat to public health. However, existing water disinfection technologies are often not only energy and chemical intensive but also inefficient at eliminating antibiotic resistance genes (ARGs). Here we show a sequential electrochemical process of ‘chemical (H2O2 pre-treatment)–physical (nanotip electroporation)–chemical (•OH injection)’ that is highly effective in inactivating ARB and removing ARGs. The bacteria are first pre-treated by H2O2 generated via two-electron water oxidation in the SnO2−x/TiO2 anode region to reduce the defences of bacterial outer walls against electroporation. Then, the ‘softened’ and ‘weakened’ bacteria are easily punctured by electroporation in the Pd-Au/TiO2 cathode region and by synchronously injected abundant •OH generated via three-electron oxygen reduction. Bacterial inclusions, including nuclear body and cytoplasm, are effectively decomposed by •OH oxidation, resulting in the destruction of the entire cell structure from the inside out. This bactericidal mechanism of synergetic physical damage and chemical oxidation inactivated >99.9999% of ARB and removed ~99% of ARGs at short retention time (~16 s), high flux (~4.5 m3 h−1 m−2) and low energy consumption (~42.4 Wh m−3) over 15 days of continuous operation. This approach may act as an alternative to meet the urgent need for efficient and residue-free water disinfection.

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Fig. 1: Synthesis and characterization of electrodes.
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Fig. 2: Electrochemical performance analyses of electrodes.
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Fig. 3: Inactivation efficiency.
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Fig. 4: Thoroughness of disinfection.
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Fig. 5: Disinfection mechanism.
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Data availability

The data generated in this study are provided in the main text, Methods or Supplementary Information. Source data are provided with this paper.

References

  1. Shannon, M. A. et al. Science and technology for water purification in the coming decades. Nature 452, 301–310 (2008).

    Article  PubMed  CAS  Google Scholar 

  2. Bogler, A. et al. Rethinking wastewater risks and monitoring in light of the COVID-19 pandemic. Nat. Sustain. 3, 981–990 (2020).

    Article  Google Scholar 

  3. Wu, T. et al. Solar-driven efficient heterogeneous subminute water disinfection nanosystem assembled with fingerprint MoS2. Nat. Water 1, 462–470 (2023).

    Article  Google Scholar 

  4. Alvarez, P. J. J., Chan, C. K., Elimelech, M., Halas, N. J. & Villagán, D. Emerging opportunities for nanotechnology to enhance water security. Nat. Nanotechnol. 13, 634–641 (2018).

    Article  PubMed  CAS  Google Scholar 

  5. Liu, H., Huang, W., Yu, Y. & Chen, D. Lightning-rod effect on nanowire tips reinforces electroporation and electrochemical oxidation: an efficient strategy for eliminating intracellular antibiotic resistance genes. ACS Nano 17, 3037–3046 (2023).

    Article  PubMed  CAS  Google Scholar 

  6. Gupta, A., Mumtaz, S., Li, C. H., Hussain, I. & Rotello, V. M. Combatting antibiotic-resistant bacteria using nanomaterials. Chem. Soc. Rev. 48, 415–427 (2019).

    Article  PubMed  PubMed Central  Google Scholar 

  7. Mauter, M. S. et al. The role of nanotechnology in tackling global water challenges. Nat. Sustain. 1, 166–175 (2018).

    Article  Google Scholar 

  8. Guo, Y. H., Dundas, C. M., Zhou, X. Y., Johnston, K. P. & Yu, G. H. Molecular engineering of hydrogels for rapid water disinfection and sustainable solar vapor generation. Adv. Mater. 33, 2102994 (2021).

    Article  CAS  Google Scholar 

  9. Liu, F. Y. et al. Catalyst-free periodate activation by solar irradiation for bacterial disinfection: performance and mechanisms. Environ. Sci. Technol. 56, 4413–4424 (2022).

    Article  PubMed  CAS  Google Scholar 

  10. Chen, Y., Ji, Q. H., Zhang, G., Liu, H. J. & Qu, J. H. Synergetic lipid extraction with oxidative damage amplifies cell-membrane-destructive stresses and enables rapid sterilization. Angew. Chem. Int. Ed. 60, 7744–7751 (2021).

    Article  CAS  Google Scholar 

  11. Richards, T. et al. A residue-free approach to water disinfection using catalytic in situ generation of reactive oxygen species. Nat. Catal. 4, 575–585 (2021).

    Article  CAS  Google Scholar 

  12. Luo, X. F., Li, W. G., Liang, Z. X., Liu, Y. F. & Fan, D. E. Portable bulk-water disinfection by live capture of bacteria with divergently branched porous graphite in electric fields. ACS Nano 17, 10041–10054 (2023).

    Article  PubMed  CAS  Google Scholar 

  13. Liu, F. Y. et al. Periodate activation by pyrite for the disinfection of antibiotic-resistant bacteria: performance and mechanisms. Water Res. 230, 119508 (2023).

    Article  PubMed  CAS  Google Scholar 

  14. Wang, Y., Lu, Y. W. & Liu, H. Nanowire electroporation-induced cell pores on antibiotic-resistant bacteria to promote chlorine permeation for eliminating intracellular antibiotic resistance genes. Chem. Eng. J. 479, 147801 (2024).

    Article  CAS  Google Scholar 

  15. Vikesland, P. J. et al. Toward a comprehensive strategy to mitigate dissemination of environmental sources of antibiotic resistance. Environ. Sci. Technol. 51, 13061–13069 (2017).

    Article  PubMed  CAS  Google Scholar 

  16. Li, J. H. et al. Electroactive ultrafiltration membrane for simultaneous removal of antibiotic, antibiotic resistant bacteria, and antibiotic resistance genes from wastewater effluent. Environ. Sci. Technol. 56, 15120–15129 (2022).

    Article  PubMed  CAS  Google Scholar 

  17. Huo, Z. Y. et al. Triboelectrification induced self-powered microbial disinfection using nanowire-enhanced localized electric field. Nat. Commun. 12, 3693 (2021).

    Article  PubMed  PubMed Central  CAS  Google Scholar 

  18. Zhou, J. F., Wang, T. & Xie, X. Locally enhanced electric field treatment (LEEFT) promotes the performance of ozonation for bacteria inactivation by disrupting the cell membrane. Environ. Sci. Technol. 54, 14017–14025 (2020).

    Article  PubMed  CAS  Google Scholar 

  19. Huo, Z. Y. et al. Synergistic nanowire-enhanced electroporation and electrochlorination for highly efficient water disinfection. Environ. Sci. Technol. 56, 10925–10934 (2022).

    Article  PubMed  CAS  Google Scholar 

  20. Wang, G. M. et al. Quantifiable relationship between antibacterial efficacy and electro-mechanical intervention on nanowire arrays. Adv. Mater. 35, 2212315 (2023).

    Article  CAS  Google Scholar 

  21. Zhou, J. F., Hung, Y.-C. & Xie, X. Making waves: pathogen inactivation by electric field treatment: from liquid food to drinking water. Water Res. 207, 117817 (2021).

    Article  PubMed  CAS  Google Scholar 

  22. Zhang, J. K. et al. Impact of reactive oxygen species on cell activity and structural integrity of Gram-positive and Gram-negative bacteria in electrochemical disinfection system. Chem. Eng. J. 451, 138879 (2023).

    Article  CAS  Google Scholar 

  23. Zeng, Y. C. & Wu, G. Electrocatalytic H2O2 generation for disinfection. Chin. J. Catal. 42, 2149–2163 (2021).

    Article  CAS  Google Scholar 

  24. Zhang, J., Zhang, G., Lan, H. C., Liu, H. J. & Qu, J. H. Selective oxygen activation to reactive oxygen species on a carbon layer-encapsulated CuxO electrocatalyst for water purification. Environ. Sci. Technol. 57, 1134–1143 (2023).

    Article  PubMed  CAS  Google Scholar 

  25. Qu, S. Y., Wu, H. & Ng, Y. H. Thin zinc oxide layer passivating bismuth vanadate for selective photoelectrochemical water oxidation to hydrogen peroxide. Small 19, 2300347 (2023).

    Article  CAS  Google Scholar 

  26. Zhang, K. et al. Near-complete suppression of oxygen evolution for photoelectrochemical H2O oxidative H2O2 synthesis. J. Am. Chem. Soc. 142, 8641–8648 (2020).

    Article  PubMed  CAS  Google Scholar 

  27. Xie, L. B. et al. The strong metal-support interactions induced electrocatalytic three-electron oxygen reduction to hydroxyl radicals for water treatment. Proc. Natl Acad. Sci. USA 120, e2307989120 (2023).

    Article  PubMed  PubMed Central  CAS  Google Scholar 

  28. Song, R. et al. Highly efficient degradation of persistent pollutants with 3D nanocone TiO2-based photoelectrocatalysis. J. Am. Chem. Soc. 143, 13664–13674 (2021).

    Article  PubMed  CAS  Google Scholar 

  29. Liu, J. L. et al. Oxygen vacancy management for high-temperature mesoporous SnO2 electron transport layers in printable perovskite solar cells. Angew. Chem. Int. Ed. 61, e202202012 (2022).

    Article  CAS  Google Scholar 

  30. Zhang, J. et al. Synchronous reduction-oxidation process for efficient removal of trichloroacetic acid: H* initiates dechlorination and •OH is responsible for removal efficiency. Environ. Sci. Technol. 53, 14586–14594 (2019).

    Article  PubMed  CAS  Google Scholar 

  31. Chen, Y. F. et al. Facet-engineered TiO2 drives photocatalytic activity and stability of supported noble metal clusters during H2 evolution. Nat. Commun. 14, 6165 (2023).

    Article  PubMed  PubMed Central  CAS  Google Scholar 

  32. Gill, T. M., Vallez, L. & Zheng, X. L. The role of bicarbonate-based electrolytes in H2O2 production through two-electron water oxidation. ACS Energy Lett. 6, 2854–2862 (2021).

    Article  CAS  Google Scholar 

  33. Ou, M. et al. Tailored BiVO4 photoanode hydrophobic microenvironment enables water oxidative H2O2 accumulation. Adv. Sci. 10, 2300169 (2023).

    Article  CAS  Google Scholar 

  34. Zeng, H. B. et al. pH-independent production of hydroxyl radical from atomic H*-mediated electrocatalytic H2O2 reduction: a green Fenton process without byproducts. Environ. Sci. Technol. 54, 14725–14731 (2020).

    Article  PubMed  CAS  Google Scholar 

  35. Xiao, F. et al. Selective electrocatalytic reduction of oxygen to hydroxyl radicals via 3-electron pathway with FeCo alloy encapsulated carbon aerogel for fast and complete removing pollutants. Angew. Chem. Int. Ed. 60, 10375–10383 (2021).

    Article  CAS  Google Scholar 

  36. Xu, X. M. et al. Revealing *OOH key intermediates and regulating H2O2 photoactivation by surface relaxation of Fenton-like catalysts. Proc. Natl Acad. Sci. USA 119, e2205562119 (2022).

    Article  PubMed  PubMed Central  CAS  Google Scholar 

  37. Wang, H. et al. Oxygen-vacancy-mediated exciton dissociation in BiOBr for boosting charge-carrier-involved molecular oxygen activation. J. Am. Chem. Soc. 140, 1760–1766 (2018).

    Article  PubMed  CAS  Google Scholar 

  38. Zhang, J. & Qu, S. Y. Synergetic multiple free radicals lower the organohalide conversion barrier and potentiate effective contaminant mineralization. Appl. Catal. B 343, 123554 (2024).

    Article  CAS  Google Scholar 

  39. Xie, L. B. et al. Pauling-type adsorption of O2 induced electrocatalytic singlet oxygen production on N–CuO for organic pollutants degradation. Nat. Commun. 13, 5560 (2022).

    Article  PubMed  PubMed Central  CAS  Google Scholar 

  40. Jin, L. L. et al. Microenvironment-activated nanozyme-armed bacteriophages efficiently combat bacterial infection. Adv. Mater. 35, 2301349 (2023).

    Article  CAS  Google Scholar 

  41. Piggot, T. J., Holdbrook, D. A. & Khalid, S. Electroporation of the E. coli and S. aureus membranes: molecular dynamics simulations of complex bacterial membranes. J. Phys. Chem. B 115, 13381–13388 (2011).

    Article  PubMed  CAS  Google Scholar 

  42. Garde, S., Chodisetti, P. K. & Reddy, M. Peptidoglycan: structure, synthesis, and regulation. EcoSal Plus 9, eESP-0010-2020 (2021).

    Article  PubMed  PubMed Central  Google Scholar 

  43. Pasquina-Lemonche, L. et al. The architecture of the Gram-positive bacterial cell wall. Nature 582, 294–297 (2020).

    Article  PubMed  PubMed Central  CAS  Google Scholar 

  44. Ibsen, K. N. et al. Mechanism of antibacterial activity of choline-based ionic liquids (CAGE). ACS Biomater. Sci. Eng. 4, 2370–2379 (2018).

    Article  PubMed  CAS  Google Scholar 

  45. Wang, T. & Xie, X. Nanosecond bacteria inactivation realized by locally enhanced electric field treatment. Nat. Water 1, 104–112 (2023).

    Article  Google Scholar 

  46. Zhang, J., Qu, S. Y., Li, B., Li, X. Y. & Lin, L. In-situ investigation into the dynamic evolution of electrode surface H* and H* mediated pH-independent and residue-free electro-Fenton process. Chem. Eng. J. 473, 145494 (2023).

    Article  CAS  Google Scholar 

  47. Yang, C. W. et al. Interfacial O2 accumulation affects microenvironment in carbon-based electrocatalysts for H2O2 production. ACS Energy Lett. 7, 4398–4407 (2022).

    Article  CAS  Google Scholar 

  48. Zhang, J. et al. Synergetic oxidation of the hydroxyl radical and superoxide anion lowers the benzoquinone intermediate conversion barrier and potentiates effective aromatic pollutant mineralization. Environ. Sci. Technol. 57, 12117–12126 (2023).

    Article  PubMed  CAS  Google Scholar 

  49. Zhang, J., Qu, S. Y., Li, B., Li, X. Y. & Lin, L. Nitrogen coordination modulation of single-atom CoN4 enables dual-active-sites catalyst featuring synergistic organics adsorption and peroxymonosulfate activation. Chem. Eng. J. 468, 143593 (2023).

    Article  CAS  Google Scholar 

  50. Zhang, J. et al. Carbon nanodot-modified FeOCl for photo-assisted Fenton reaction featuring synergistic in-situ H2O2 production and activation. Appl. Catal. B 266, 118665 (2020).

    Article  CAS  Google Scholar 

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Acknowledgements

We gratefully acknowledge the financial support by the National Natural Science Foundation of China (52300096 for J.Z. and 52270128 for X.-Y.L.), the China Postdoctoral Science Foundation (2023M731933 for J.Z.), the China State-sponsored Postdoctoral Researcher Program Grade B for J.Z., the Guangdong Basic and Applied Basic Research Foundation (2023A1515011734 for L. Lin), the Shenzhen Municipal Science and Technology Innovation Council of the Shenzhen Government (KCXFZ20211020163556020 for X.-Y.L.) and the ‘Shuimu Tsinghua Scholar’ Program of Tsinghua University for J.Z.

Author information

Authors and Affiliations

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

    Jun Zhang, Ruiquan Yu, Wutong Chen, Lin Lin, Bing Li & Xiao-Yan Li

  2. Advanced Interdisciplinary Institute of Environment and Ecology, Guangdong Provincial Key Laboratory of Wastewater Information Analysis and Early Warning, Beijing Normal University, Zhuhai, China

    Jun Zhang & Li Ling

  3. Macau Institute of Materials Science and Engineering, Faculty of Innovation Engineering, Macau University of Science and Technology, Taipa, Macau SAR

    Songying Qu

  4. Environmental Engineering Research Centre, Department of Civil Engineering, The University of Hong Kong, Pokfulam, Hong Kong SAR

    Xiao-Yan Li

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  1. Jun Zhang
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Contributions

J.Z. and S.Q. conceived the idea and designed the experiments. J.Z., S.Q. and R.Y. implemented the experimental setup and conducted the experiments. J.Z., S.Q. and W.C. carried out the DFT calculations. J.Z., S.Q. and L. Ling carried out the COMSOL (COMSOL Co., Ltd) Multiphysics simulations. J.Z., S.Q. and B.L. carried out the MD simulations. J.Z., S.Q., L. Lin and X.-Y.L. wrote the paper. J.Z., L. Lin and X.-Y.L. supervised the work. All the authors discussed the results and commented on the paper.

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Correspondence to Jun Zhang, Songying Qu, Lin Lin or Xiao-Yan Li.

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Nature Water thanks Xing Xie and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Zhang, J., Qu, S., Yu, R. et al. Synergetic physical damage and chemical oxidation for highly efficient and residue-free water disinfection. Nat Water 2, 1226–1237 (2024). https://doi.org/10.1038/s44221-024-00344-0

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