School of Environmental Engineering, Wuhan Textile University, Wuhan 430073, China; School of Environmental and Biological Engineering, Nanjing University of Science and Technology, Nanjing 210094, China.
School of Environmental Engineering, Wuhan Textile University, Wuhan 430073, China; College of Resources and Environment, University of Chinese Academy of Sciences, Beijing 100049, China.
J Hazard Mater. 2021 Apr 5;407:124393. doi: 10.1016/j.jhazmat.2020.124393. Epub 2020 Nov 2.
The present research systematically investigates the atenolol (ATL) degradation in integrated UV/Ozone (O)/peroxymonosulfate (PMS) process focusing on the synergistic mechanism, reaction kinetics, pollutant degradation pathway and antibacterial activity. The results manifested that the integrated UV/O/PMS process showed the noteworthy superiority to ATL degradation compared with UV/PMS, UV/O and O/PMS systems. Simultaneously, the impacts of operating parameters like PMS dosage, initial ATL concentration, solution pH and water matrix were comprehensively explored. The ATL elimination efficiency increased linearly with PMS dose and significantly enhanced in alkaline conditions. The OH and SO were the primary reactive radicals for ATL oxidation in UV/O/PMS system based on the radical scavenging experiments and electron paramagnetic resonance characterization. Besides, a simplified kinetic model on the basis of the dominant reactions and the steady-state assumption was established to foretell the relative contributions of reactive oxidants for ATL elimination in UV/O/PMS process. Main transformation products were determined via UPLC-QTOF-MS to infer the possible degradation pathways of ATL. Furthermore, the UV/O/PMS process could distinctly mitigate the antibacterial activity of ATL and its intermediates to E. coli and B. subtilis. Our findings may have critical implications for the development of novel oxidation processes for recalcitrant contaminants mitigation in water purification.
本研究系统考察了在集成 UV/Ozone（O）/过一硫酸盐（PMS）工艺中，关注协同机制、反应动力学、污染物降解途径和抗菌活性的阿替洛尔（ATL）降解。结果表明，与 UV/PMS、UV/O 和 O/PMS 系统相比，集成 UV/O/PMS 工艺对 ATL 降解具有显著优势。同时，全面探讨了操作参数如 PMS 剂量、初始 ATL 浓度、溶液 pH 值和水基质的影响。ATL 的去除效率随 PMS 剂量线性增加，并在碱性条件下显著增强。基于自由基清除实验和电子顺磁共振表征，确定了 OH 和 SO 是 UV/O/PMS 体系中 ATL 氧化的主要反应性自由基。此外，根据主要反应和稳态假设，建立了简化的动力学模型，以预测 UV/O/PMS 工艺中各种反应性氧化剂对 ATL 去除的相对贡献。通过 UPLC-QTOF-MS 确定主要转化产物，推断 ATL 的可能降解途径。此外，UV/O/PMS 工艺可明显减轻 ATL 及其中间产物对大肠杆菌和枯草芽孢杆菌的抗菌活性。我们的研究结果可能对开发新型氧化工艺以减轻水中难降解污染物的处理具有重要意义。
