基于金属单原子/原子簇分散多孔碳电极的电Fenton过程及强化机理

毒性有机污染物(如持久性有毒物质PTS等)的去除是水处理领域重点和难点课题。Fenton反应可产生高活性·OH，能有效分解毒性有机污染物，但存在反应须在酸性条件下进行，产生铁泥，造成二次污染等问题。电Fenton技术能够克服上述问题，但原位产生H2O2的效率低和H2O2活化生成·OH效率低是实用化的瓶颈。本项目以提高H2O2产率和电Fenton反应效率为目标，拟设计、制备具有高效、稳定催化O2还原产H2O2、活化H2O2生成·OH的金属单原子/原子簇分散多孔碳电极，揭示单原子/原子簇催化O2还原产H2O2、活化H2O2生成·OH的强化机理与多孔碳协同作用机制，构建电Fenton水处理装置，通过实际废水处理评价其毒性污染物分解和毒性削减性能以及经济性和实用性。本项目为设计制备高效、低耗、稳定的电Fenton电极材料提供理论依据，为推动电Fenton技术从基础研究向工程应用的转化提供理论基础。

The removal of toxic organic pollutants，such as persistent toxic substances (PTS), which are strongly resistant to conventional biological and physiochemical technologies, is a big challenge in the field of water and wastewater treatment. Fenton reaction, as an advanced oxidation process (AOPs), is promising for the removal of toxic organic pollutants. Fenton reaction can produce highly active oxidation radicals, namely hydroxyl radicals from H2O2 conversion, which can oxidize and mineralize most organic pollutants. Nevertheless, the traditional homogeneous Fenton reaction is restricted to acidic conditions (pH < 3) and will produce large amount of ferric sludge, which are the main obstacles in the practical application. Electro-Fenton reaction could overcome these obstacles, and become an attractive technology for degradation of organic pollutants. However, it is still suffering from low efficiency, which leads to its meaningless for practical application. In the Electro-Fenton reaction, the efficiency of pollutants degradation is highly dependent on the yield of H2O2, which is electrochemically generated in situ from O2 reduction on the cathode, and conversion of H2O2 to hydroxyl radicals, which can degrade organic pollutants. Aiming at improving the yield of H2O2 and the efficiency of electro-Fenton, this project is going to (1) design and fabricate porous carbon electrode with atomically dispersed metal sites for highly efficient and stable in situ H2O2 production from O2 reduction and hydroxyl radical generation from H2O2 conversion, (2) elucidate the mechanism of Electro-Fenton reaction enhancement by porous carbon with atomically dispersed metal sites, (3) develop relevant water treatment devices to explore the feasibility of their practical applications, and evaluate their performance in selected PTS or PPCPs removal and toxicity reduction. This work will provide a new insight into design of highly efficient and low-cost electro-Fenton catalysts, and provide theoretical basis for the practical application of the electro-Fenton reaction in water and wastewater treatment.