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主办单位:煤炭科学研究总院有限公司、中国煤炭学会学术期刊工作委员会
过氧化物微调控铜铈双反应中心催化剂诱发氧活化驱动水净化
  • Title

    Peroxide-Micro-Modulated Dual Reaction Center Catalyst InducingOxygen Activation for Water Purification

  • 作者

    方谦杨东旋孙英涛付紫薇吴沅忠曹文锐胡春吕来

  • Author

    FANG Qian;YANG Dongxuan;SUN Yingtao;FU Ziwei;WU Yuanzhong;CAO Wenrui;HU Chun;LYU Lai

  • 单位

    广州大学大湾区环境研究院珠江三角洲水质安全与保护教育部重点实验室广州大学环境科学与工程学院香港城市大学化学系

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

    水中难降解有机污染物结构稳定且具有生物毒性,严重威胁水生态安全和人类健康。传统水处理工艺往往需要依靠大量外部能源和氧化剂来实现污染物的降解,这成为水净化难点。本文提出通过一种表面电子非均匀分布的铜铈氧化物双反应中心(DualReactionCenters,DRCs)催化剂(CCO)与微量诱发剂作用驱动水中内源物质能量利用创新策略实现低能耗水净化。结构表征和密度泛函理论(DFT)计算证实,Cu—O—Ce键桥的形成诱发表面电子极化分布,从而提高了催化活性。在微量过一硫酸盐(PMS)调控下,在5min内CCO体系即可实现多种难降解有机污染物(如酸性橙7和环丙沙星等)100%去除,且在宽pH范围(3~11)及复杂阴离子共存条件下均表现出优异的适应性和稳定性。对于实际餐厨废水,CCO体系仍能在5min内实现快速净化。结果表明,微量PMS能够诱发水中惰性溶解氧(DO)在CCO表面富电子中心“1电子”定向微活化,驱动污染物在贫电子中心供电子裂解,有效提升体系中污染物能量的利用,避免了DO多电子还原过程中电子和能量的损耗,为开发低碳、高效的水处理技术提供了新思路。

  • Abstract

    Refractory  organic  pollutants  pose  a  serious  threat  to  both  water  ecological  security  andhuman  health  due  to  their  stable  molecular  structures  and  high  biotoxicity  to  biological  organisms.These  pollutants  resist  natural  degradation  processes  and  require  powerful  chemical  oxidation  foreffective  destruction,  often  consuming  large  amounts  of  energy  and  oxidant.  This  has  become  anecessary 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 acopper-cerium oxide dual-reaction-center catalyst (CCO) with trace activators. Characterization resultsand density functional theory (DFT) calculations confirm that the formation of Cu—O—Ce bondingbridges  leads  to  a  polarized  electron  distribution  on  the  catalyst  surface,  creating  electron-rich  Cecenters and electron-poor Cu/O centers. This enhances pollutant removal efficiency in the CCO system.Under trace amounts of peroxymonosulfate (PMS) modulation, the CCO system can completely removevarious  refractory  organic  pollutants  (such  as  acid  orange  7  and  ciprofloxacin)  within  5  minutes,exhibiting excellent adaptability and stability across a wide pH range (3–11) and under complex anioncoexistence conditions. Meanwhile, the CCO system also exhibits excellent adaptability and catalyticactivity across a wide pH range (3–11) and in the presence of various anions (e.g., , , , and Cl). Notably, the CCO/PMS system achieved a pollutant removal rate of over 70% after 288hours of continuous operation in a laboratory pilot plant. This demonstrates the exceptional stability ofthe  CCO  system,  making  it  a  promising  candidate  for  practical  application.  Furthermore,  the  CCOsystem can rapidly remove organics from complex kitchen wastewater within 5 minutes, aided by traceamounts of PMS. In this reaction, PMS plays a non-traditional role, micro-regulating the distortion ofwater 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,  drivingcontinuous electron donation from pollutants at the electron-poor Cu/O centers. This avoids energy lossin the multi-electron reduction process of DO, enhances the utilization of intrinsic pollutant electronsand energy, and achieves high-efficiency, low-consumption water purification. This study provides newideas  for  developing  novel  water  treatment  technologies  based  on  the  utilization  of  endogenoussubstances and energy of wastewater.

  • 关键词

    过氧化物微调控双反应中心溶解氧活化低消耗水净化

  • KeyWords

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

  • 基金项目(Foundation)
    广东省重点领域研发计划项目纳米科技专项(2023B0101200004);国家自然科学基金资助项目(面上52470069);广州大学研究生创新能力培养计划(JCCX2024-058)
  • DOI
  • 引用格式
    方谦,杨东旋,孙英涛,等.过氧化物微调控铜铈双反应中心催化剂诱发氧活化驱动水净化[J].能源环境保护,2025,39(1):135−144.
  • Citation
    FANG Qian, YANG Dongxuan, SUN Yingtao, et al. Peroxide-Micro-Modulated Dual Reaction Center Cata-lyst Inducing Oxygen Activation for Water Purification[J]. Energy Environmental Protection, 2025, 39(1):135−144.
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