Lu Zhicong, Zhang Peng, Hu Chun, Li Fan
Key Laboratory for Water Quality and Conservation of the Pearl River Delta, Ministry of Education, Institute of Environmental Research at Greater Bay, Guangzhou University, Guangzhou 510006, China.
iScience. 2022 Aug 12;25(9):104930. doi: 10.1016/j.isci.2022.104930. eCollection 2022 Sep 16.
Persulfate-based nonradical oxidation processes are appealing in water treatment for the efficient and selective degradation of trace contaminants in complex water matrices. However, there is still lacking of systematic understanding of the relationship between multiple nonradical pathways and the active sites of catalyst. Herein, a single-atom Cu catalyst with saturated Cu-N sites on a carbon substrate (SA-Cu-NC) was constructed to activate peroxymonosulfate (PMS), which exhibited high catalytic performance and selectivity for pollutant degradation in different water conditions. Combined with the results of density functional theory (DFT) calculations, the electron-rich area around Cu site and the electron-poor area around C site in the saturated Cu-N configuration could efficiently adsorb and activate PMS, which promoted pollutant degradation through the oxidation of singlet oxygen (O) and electron transfer process, respectively. This study advances the understanding of the saturated coordination structure of metals and the superiority of multiple nonradical pathways in wastewater treatment.
基于过硫酸盐的非自由基氧化过程在水处理中颇具吸引力，可有效且选择性地降解复杂水基质中的痕量污染物。然而，目前仍缺乏对多种非自由基途径与催化剂活性位点之间关系的系统认识。在此，构建了一种在碳基底上具有饱和Cu-N位点的单原子Cu催化剂（SA-Cu-NC）来活化过一硫酸盐（PMS），该催化剂在不同水质条件下对污染物降解表现出高催化性能和选择性。结合密度泛函理论（DFT）计算结果，饱和Cu-N构型中Cu位点周围的富电子区域和C位点周围的贫电子区域可有效吸附并活化PMS，分别通过单线态氧（O）氧化和电子转移过程促进污染物降解。本研究推进了对金属饱和配位结构以及多种非自由基途径在废水处理中的优势的理解。
