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Peroxide-micro-modulated dual reaction center catalyst inducing oxygen activation for water purification

Received Date:2024-11-28 Revised Date:2024-12-23 Accepted Date:2024-12-25

DOI:10.20078/j.eep.20250102

Abstract:Refractory organic pollutants pose a serious threat to both water ecological security and human health due to their stab... Open+
Abstract:Refractory organic pollutants pose a serious threat to both water ecological security and human health due to their stable molecular structures and high biotoxicity to biological organisms. These pollutants resist natural degradation processes and require powerful chemical oxidation for effective destruction, often consuming large amounts of energy and oxidant. This has become a necessary approach for conventional wastewater treatment. Herein, we propose a novel strategy for low-energy water purification by utilizing the energy of endogenous substances through the interaction of a copper-cerium oxide dual-reaction-center catalyst (CCO) with trace amounts of peroxymonosulfate (PMS). Characterization results and density functional theory (DFT) calculations confirm that the formation of Cu—O—Ce bonding bridges leads to a polarized electron distribution on the catalyst surface, creating electron-rich Ce centers and electron-poor Cu/O centers. This enhances pollutant removal efficiency in the CCO system. Under natural conditions, with the addition of trace amounts of PMS micro-modulation, various refractory organic pollutants, including acid orange 7 (AO7), ciprofloxacin (CIP), phenytoin (PHT), and bisphenol A (BPA), are removed completely within 5 min in the CCO system. Meanwhile, the CCO system also exhibits excellent adaptability and catalytic activity across a wide pH range (3-11) and in the presence of various anions (e.g., HPO2 4 − SO2 4 − HCO− 3 NO− 3 and Cl−). Notably, the CCO/PMS system achieved a pollutant removal rate of over 70% after 288 hours of continuous operation in a laboratory pilot plant. This demonstrates the exceptional stability of the CCO system, making it a promising candidate for practical application. Furthermore, the CCO system can rapidly remove organics from complex kitchen wastewater within 5 minutes, aided by trace amounts of PMS. In this reaction, PMS plays a non-traditional role, micro-regulating the distortion of water molecules′ hydrogen-bond network on the CCO surface. This induces the "one-electron" micro-reduction of naturally dissolved oxygen (DO) molecules at the electron-rich Ce center, driving continuous electron donation from pollutants at the electron-poor Cu/O centers. This avoids energy loss in the multi-electron reduction process of DO, enhances the utilization of intrinsic pollutant electrons and energy, and achieves high-efficiency, low-consumption water purification. This study provides new ideas for developing novel water treatment technologies based on the utilization of endogenous substances and energy of wastewater. Close-

Authors:

  • FANG Qian1
  • YANG Dongxuan1
  • SUN Yingtao1
  • FU Ziwei2
  • WU Yuanzhong2
  • CAO Wenrui1,3,*
  • HU Chun1
  • LYU Lai1,2

Units

  • 1.  Key Laboratory for Water Quality and Conservation of the Pearl River Delta, Ministry of Education, Institute of Environmental Research at Greater Bay, Guangzhou University
  • 2.  School of Environmental Science and Engineering, Guangzhou University
  • 3.  Department of Chemistry, City University of Hong Kong

Keywords

  • Peroxide micro modulated
  • Dual reaction centers
  • Dissolved oxygen activation
  • Low consumption
  • Water purification

Citation

FANG Qian, YANG Dongxuan, SUN Yingtao, FU Ziwei, WU Yuanzhong, CAO Wenrui, HU Chun, LYU Lai. Peroxide-micro-modulated dual reaction center catalyst inducing oxygen activation for water purification[J/OL]. Energy Environmental Protection: 1-10[2025-01-09]. https://doi.org/10.20078/j.eep.20250102.

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