State Key Laboratory of Pollution Control and Resources Reuse(Tongji University), College of EnvironmentalScience and Engineering, Tongji University
Shanghai Institute of PollutionControl and Ecological Security

电催化反硝化是处理硝酸盐废水技术之一。 本文综述了电催化反硝化的最新研究进展,分析了电催化反硝化直接电子转移和原子氢(H∗)介导间接还原两种反应机理,总结了电催化反硝化的决速步是将 NO-3还原为 NO-2以及决定产物选择性的关键中间体是 NO。 在此基础上,总结了元素掺杂方法及其对电极材料催化活性中心和电催化反硝化反应路径的调控效应,提出了元素掺杂是提高电极材料催化活性、产物选择性和长期稳定性的有效手段。 此外,还讨论了其他因素如水质特征、运行参数等对电催化反硝化效果的影响,明确了水中共存卤素离子如 Cl- 和 Br- 等可显著提高 N2选择性以及大多数电极材料在中性条件下还原效果最佳。 面向日益增长的硝酸盐废水处理需求,指出了电能消耗高和实际废水水质成分复杂导致副反应多是限制电催化反硝化大规模应用的关键瓶颈。 由此,展望了电催化反硝化技术研究未来需要针对多种实际废水的理化性质开展长期中试试验,除了提高还原速率和产物选择性外,还要重点关注电能消耗并对处理尾水的安全性进行监测,以促进电催化反硝化技术的进一步发展和实际应用。

Electrocatalytic denitrification is one of the promising technologies for the treatment of nitratewastewater. This review comprehensively summarizes the recent advances in electrocatalytic denitrifica⁃tion. Two reaction mechanisms of direct electron transfer and atomic hydrogen (H∗)-mediated indirectreduction in electrocatalytic denitrification are analyzed. It is concluded that the rate-limiting step ofelectrocatalytic denitrification is the reduction of NO3 to NO2 and the key intermediate determiningproduct selectivity is NO. On this basis, the element-doping method and its regulation effects on thecatalytic active centers and the electrocatalytic denitrification pathways are summarized, and it is sug⁃gested that element doping is an effective method to improve the catalytic activity, product selectivityand long-term stability of electrode materials. In addition, the influence of other factors such as waterquality characteristics and operating parameters on the electrocatalytic denitrification performance is dis⁃cussed. It is confirmed that the coexistence of halogen ions in water, such as Cl- and Br-, can signifi⁃cantly improve the N2 selectivity, and most electrode materials exhibit- the best performance underneutral conditions. Facing the increasing demand of nitrate wastewater treatment, it is pointed out thatthe key bottlenecks limiting the large-scale application of electrocatalytic denitrification are the high e⁃lectric energy consumption and the complex composition of the actual wastewater which leads to side re⁃actions. Therefore, it is expected that the future research of electrocatalytic denitrification technologyneeds to conduct long-term pilot-scale tests based on the physicochemical properties of various actualwastewater. In addition to improving the reduction rate and product selectivity, it is also necessary topay attention to the electric energy consumption and monitor the safety of treated water to facilitate thefurther development and practical application of electrocatalytic denitrification technology.

国家自然科学基金资助项目(22276138);上海市国际科技合作项目(22230712800);污染控制与资源化研究国家重点实验室交叉研究课题资助(2022-4-ZD-07)

焦明硕,徐斌成,罗泽溪, 等. 元素掺杂材料在电催化反硝化中的研究进展[J]. 能源环境保护, 2023, 37(5): 25-35.

JIAO Mingshuo, XU Bincheng, LUO Zexi, et al. Progress in electrocatalytic denitrification using element-dopedmaterials[J]. Energy Environmental Protection, 2023, 37(5): 25-35.