Guangdong Provincial Key Laboratory of Petrochemcial Pollution Processes and Control, School of Environmental Science and Engineering, Guangdong University of Petrochemical Technology, Maoming, Guangdong 525000, China; College of Environmental Science and Engineering, Hunan University and Key Laboratory of Environmental Biology and Pollution Control (Hunan University), Ministry of Education, Changsha, Hunan 410082, China; Maoming Engineering Research Center for Organic Pollution Control, Academy of Environmental and Resource Sciences, Guangdong University of Petrochemical Technology, Maoming, Guangdong 525000, China.
Guangdong Provincial Key Laboratory of Petrochemcial Pollution Processes and Control, School of Environmental Science and Engineering, Guangdong University of Petrochemical Technology, Maoming, Guangdong 525000, China; College of Environmental Science and Engineering, Hunan University and Key Laboratory of Environmental Biology and Pollution Control (Hunan University), Ministry of Education, Changsha, Hunan 410082, China; Maoming Engineering Research Center for Organic Pollution Control, Academy of Environmental and Resource Sciences, Guangdong University of Petrochemical Technology, Maoming, Guangdong 525000, China; Hunan Provincial Environmental Protection Engineering Center for Organic Pollution Control of Urban Water and Wastewater, Changsha, Hunan 410001, China.
J Environ Sci (China). 2022 May;115:330-340. doi: 10.1016/j.jes.2021.08.002. Epub 2021 Aug 21.
Nonradical reaction driven by peroxymonosulfate (PMS) based advanced oxidation processes has drawn widespread attention in water treatment due to their inherent advantages, but the degradation behavior and mechanism of organic pollutants are still unclear. In this study, the performance, intermediates, mechanism and toxicity of tetracycline (TC) degradation were thoroughly examined in the constructed magnetic nitrogen-doped porous carbon/peroxymonosulfate (Co-N/C-PMS) system. The results showed that 85.4% of TC could be removed within 15 min when Co-N/C and PMS was simultaneously added and the degradation rate was enhanced by 3.4 and 14.7 folds compared with Co-N/C or PMS alone, respectively. Moreover, the performance of Co-N/C was superior to that of most previously reported catalysts. Many lines of evidence indicated that Co-N/C-PMS system was a singlet oxygen-dominated nonradical reaction, which was less interfered by pH and water components, and displayed high adaptability to actual water bodies. Subsequently, the degradation process was elaborated on the basis of three-dimensional excitation-emission matrix spectra and liquid chromatography-mass spectrometry. At last, the toxicity of treated TC was greatly reduced by using microalgae Coelastrella sp. as ecological indicator. This study provides a promising approach based on singlet oxygen-dominated nonradical reaction for eliminating TC in water treatment.
基于过一硫酸盐（PMS）的非自由基反应的高级氧化过程因其固有优势在水处理中引起了广泛关注，但有机污染物的降解行为和机制仍不清楚。在这项研究中，在构建的磁性氮掺杂多孔碳/过一硫酸盐（Co-N/C-PMS）体系中，彻底研究了四环素（TC）降解的性能、中间体、机制和毒性。结果表明，当同时添加 Co-N/C 和 PMS 时，TC 可在 15 分钟内去除 85.4%，与单独的 Co-N/C 或 PMS 相比，降解速率分别提高了 3.4 倍和 14.7 倍。此外，Co-N/C 的性能优于大多数先前报道的催化剂。许多证据表明，Co-N/C-PMS 体系是一种单线态氧主导的非自由基反应，受 pH 和水成分的干扰较小，对实际水体具有较高的适应性。随后，基于三维激发-发射矩阵光谱和液相色谱-质谱对降解过程进行了阐述。最后，使用微藻 Coelastrella sp. 作为生态指标，大大降低了处理后的 TC 的毒性。这项研究为基于单线态氧主导的非自由基反应的水处理中消除 TC 提供了一种有前途的方法。
