Chen Xin, Wang Yaqi, Fan Xinfei, Zhu Genwang, Liu Yanming, Quan Xie
Key Laboratory of Industrial Ecology and Environmental Engineering (Ministry of Education, China), School of Environmental Science and Technology, Dalian University of Technology, Dalian 116024, China.
College of Environmental Science and Engineering, Dalian Maritime University, Dalian 116026, China.
Sci Total Environ. 2024 Jul 1;932:173042. doi: 10.1016/j.scitotenv.2024.173042. Epub 2024 May 8.
The electro-Fenton with in situ generated O and OH is a promising method for the degradation of micropollutants. However, its application is hindered by the lack of catalysts that can efficiently generate O and OH from electrochemical oxygen reduction. Herein, N-doped stacked carbon nanosheets supported Fe single atoms (Fe-NSC) with FeN sites were designed for simultaneous generation of O and OH to enhance electro-Fenton degradation. Due to the synergistic effect of O and OH, a variety of contaminants (phenol, 2,4-dichlorophenol, sulfamethoxazole, atrazine and bisphenol A) were efficiently degraded with high kinetic constants of 0.037-0.071 min by the electro-Fenton with Fe-NSC as cathode (-0.6 V vs Ag/AgCl, pH 6). Moreover, the superior performance for electro-Fenton degradation was well maintained in a wide pH range from 3 to 10 even with interference of various inorganic salt ions. It was found that FeN sites with pyridinic N coordination were responsible for its good performance for electro-Fenton degradation. Its O yield was higher than OH yield, and the contribution of O was more significant than OH for pollutant degradation.
原位生成O和OH的电芬顿法是一种很有前景的微污染物降解方法。然而，其应用受到缺乏能从电化学氧还原高效生成O和OH的催化剂的阻碍。在此，设计了具有FeN位点的N掺杂堆叠碳纳米片负载的Fe单原子（Fe-NSC），用于同时生成O和OH以增强电芬顿降解。由于O和OH的协同作用，以Fe-NSC为阴极（相对于Ag/AgCl为-0.6 V，pH 6）的电芬顿法能高效降解多种污染物（苯酚、2,4-二氯苯酚、磺胺甲恶唑、阿特拉津和双酚A），其动力学常数高达0.037-0.071 min。此外，即使在各种无机盐离子的干扰下，电芬顿降解的优异性能在3至10的宽pH范围内也能得到很好的保持。研究发现，具有吡啶N配位的FeN位点是其电芬顿降解良好性能的原因。其O产率高于OH产率，且O对污染物降解的贡献比OH更显著。
