Key Laboratory of Pollution Process and Environmental Criteria, Ministry of Education, College of Environmental Science and Engineering, Nankai University, Tianjin, 300350, China; Tianjin Key Laboratory of Environmental Technology for Complex Trans-Media Pollution, College of Environmental Science and Engineering, Nankai University, Tianjin, 300350, China; Tianjin Advanced Water Treatment Technology International Joint Research Center, College of Environmental Science and Engineering, Nankai University, Tianjin, 300350, China.
Tianjin Fisheries Research Institute, Tianjin, 300221, China.
Chemosphere. 2022 Nov;307(Pt 4):136168. doi: 10.1016/j.chemosphere.2022.136168. Epub 2022 Aug 26.
To improve the performance and solve the restrictions of UV/chlorine process (e.g., the narrow pH application range and high disinfection by-products (DBPs) formation), a Fe assisted advanced oxidation process with electrochemically generated chlorine (UV/E-Cl/Fe) was proposed for carbamazepine (CBZ) degradation, which eliminated CBZ (5 mg/L) within 4 min under the optimal conditions. Compared with UV/electro-generated chlorine (UV/E-Cl) and anodic oxidation-chlorination/Fe (AO-Cl/Fe) processes, the apparent first-order kinetics constant in UV/E-Cl/Fe increased by 2.56 and 3.18 times respectively, and the energy consumption was lower (1.15 kWh/m-log). Simultaneously, the pH application range could be expanded to 9, and DBPs formed in this process were 17.1% less than those in UV/E-Cl. Through quenching tests, electron paramagnetic resonance (EPR) experiments, measurement of OH concentration, quantification of methyl phenyl sulfoxide (PMSO) and benzosulfone (PMSO) and processes comparison, possible CBZ degradation pathways and mechanism of UV/E-Cl/Fe were proposed, in which Fe(IV) played the dominant role in the early stage, while the production of radicals (i.e., OH and Cl) was enhanced with the increase of chlorine generation, accelerating the CBZ removal. Furthermore, this process demonstrated wide application prospect in treating various contaminants and real wastewaters. In conclusion, this study offers an effective and energy-efficient method for organic pollutants degradation.
为了提高性能并解决 UV/氯工艺的限制（例如，应用范围狭窄的 pH 值和高消毒副产物 (DBPs) 形成），提出了一种 Fe 辅助的电化学产生氯的高级氧化工艺（UV/E-Cl/Fe），用于卡马西平 (CBZ) 的降解，在最佳条件下，可在 4 分钟内消除 5mg/L 的 CBZ。与 UV/电生成氯 (UV/E-Cl) 和阳极氧化氯化/Fe (AO-Cl/Fe) 工艺相比，UV/E-Cl/Fe 中的表观一级动力学常数分别提高了 2.56 和 3.18 倍，能耗更低（1.15 kWh/m-log）。同时，pH 值应用范围可扩展至 9，且该过程形成的 DBPs 比 UV/E-Cl 少 17.1%。通过猝灭试验、电子顺磁共振 (EPR) 实验、OH 浓度测量、甲磺酸苯砜 (PMSO) 和苯磺酮 (PMSO) 的定量以及过程比较，提出了可能的 CBZ 降解途径和 UV/E-Cl/Fe 机制，其中 Fe(IV) 在早期起主导作用，而随着氯生成的增加，自由基（即 OH 和 Cl）的产生增强，加速了 CBZ 的去除。此外，该工艺在处理各种污染物和实际废水方面表现出广阔的应用前景。总之，本研究为有机污染物的降解提供了一种有效且节能的方法。
