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投稿时间:2021-08-09 修订日期:2022-09-19
投稿时间:2021-08-09 修订日期:2022-09-19
中文摘要: 糖精(Saccharin,SAC)是一种最早应用于食品、饮料、医药和饲料中的人工甜味剂,几乎不为人体和生物吸收,经排放进入水环境中,因检出频率及浓度高,衰减慢且存在毒性风险等被认定为环境新型有机污染物。本文对比了饮用水的多种预氧化工艺对水中SAC的降解效果,对UV/H2O2联用工艺降解SAC进行了动力学分析,同时,考察了氧化剂量、初始SAC浓度和水中常见共存阴离子($\mathrm{Cl}^{-}{\text{、}}\!\! \mathrm{CO}_3^{2-}{\text{、}}\!\! \mathrm{NO}_3^{-}{\text{、}}\!\!\mathrm{SO}_4^{2-} $)等因素对氧化体系降解SAC的影响。结果表明:1)氯化、单独的UV或 H2O2对SAC去除能力低,分别为21.17%、9.74%和7.69%。臭氧和UV/H2O2联用两种氧化工艺对SAC的去除效果良好,氧化接触时间30 min后降解率均高于85%,UV/H2O2联用的降解和矿化速率更快。连续臭氧维持7.10 mg/min 通量60 min可降解99%以上的SAC,与20.4 mg/L H2O2在1.46 mW/cm2 UV光强辐照60 min的效果相当。2)在对UV/H2O2联用工艺的影响因素考察中发现,H2O2投加量的增加会加快SAC的降解速率,但高浓度H2O2会抑制降解作用;UV光强的增加可促进降解反应,SAC初始浓度的增加会降低降解速率;酸性及较高温度对反应有促进作用。对糖精进行降解,UV/H2O2体系的最佳氧化条件为20.4 mg/L H2O2,1.46 mW/cm2辐照量,酸性条件(pH值3),水温30 ℃。水中常见离子对UV/H2O2降解SAC存在抑制作用,强弱次序依次为$\mathrm{NO}_3^{-}>\mathrm{SO}_4^{2-}>\mathrm{CO}_3^{2-}>\mathrm{Cl}^{-} $。3)UV/H2O2降解SAC主要通过羟基自由基(·OH)反应,降解途径可能为苯环被自由基羟基化,C—N键断裂。臭氧对SAC的降解效率较高,但氧化剂投加量较大,UV/H2O2联用可更高效地降解SAC,但能耗较高。因此仍需探索低碳、高效去除水源水中SAC等微量有机污染物的工艺。
中文关键词: UV/H2O2联用工艺 糖精 饮用水处理 氧化降解 水质安全
Abstract:Saccharin (SAC) is the earliest artificial sweetener applied as additive in food, beverage, medicine and forage. SAC is hardly digested by human body and other organisms, and discharged into the water environment mostly. Characterized with high detection frequency and concentration, outstanding persistence and toxicity risk, SAC has been recognized as an emerging organic contaminant. Focused on UV/H2O2 process, the degradation of SAC by pre-chlorine, ozonation and UV/H2O2 was compared from the aspect of degradation efficiency and kinetics. The influencing factors including oxidant dosage, UV radiation intensity, initial SAC concentration, the pH value of solution, water temperature, and common anions ($\mathrm{Cl}^{-}, \mathrm{CO}_3^{2-}, \mathrm{NO}_3^{-}, \mathrm{SO}_4^{2-} $) on the degradation of SAC in oxidation system were explored. The results were listed as follows: 1) The removal of SAC by chlorination, UV and H2O2 alone is 21.17%, 9.74% and 7.69%, respectively., while ozonation and UV/H2O2 exhibit significant degradation of SAC (as the degradation efficiency more than 85% after 30 minutes of oxidation), and faster reaction and mineralization rate in UV/H2O2 system. By ozonation with continuous flux 7.10 mg/min for 60 min, the degradation of SAC reaches the similar level as that under oxidation condition of H2O2 (20.4 mg/L) irradiated by UV intensity of 1.46 mW/cm2 for 60 min. 2) In the investigation of the influencing factors of UV/H2O2 combined process, the increase of H2O2 dosage accelerates the degradation rate of SAC, however, the over dosage of H2O2 inhibates the degradation. The increase of UV light intensity promotes the degradation, while the increase of the initial concentration of SAC decreases the degradation rate. Acidity and higher temperature promotes the reaction. The optimum oxidation conditions of UV/H2O2 system is 20.4 mg/L H2O2, 1.46 mW/cm2 UV intensity, pH 3, and the reaction water temperatureof 30 ℃. The degradation of SAC by UV/H2O2 is inhibited by common ions in water, following the sequence of $\mathrm{NO}_3^{-}>\mathrm{SO}_4^{2-}>\mathrm{CO}_3^{2-}>\mathrm{Cl}^{-} $. 3) The degradation of SAC by UV/H2O2 mainly by the hydroxyl radical, and the main pathway may be that the benzene ring is hydroxylated by the free radical and the C—N bond is broken. Although ozonation has a high degradation efficiency of SAC, the oxidant consumption is much. While UV/H2O2 treats SAC more efficiently, however, the energy consumption is higher. Therefore, it is still necessary to explore the low-carbon demand and high efficient process to remove trace organic pollutants like SAC in source water.
keywords: UV/H2O2 combined progress saccharin drinking water treatment oxidation degradation water quality safety
文章编号:202100776 中图分类号:TU991 文献标志码:
基金项目:国家自然科学基金项目(51678527; 51878582);浙江省自然科学基金项目(LY19E080019)
作者简介:第一作者:项硕(1977—),男,讲师,博士. 研究方向:水污染控制. E-mail:ljp23@zjut.edu.cn;通信作者:宋亚丽, E-mail:yali_song@sina.com
引用文本:
项硕,金雨鸿,李青松,宋亚丽,黄奕鸣,马晓雁.水中新型有机污染糖精的氧化降解及动力学分析[J].工程科学与技术,2022,54(5):210-217.
XIANG Shuo,JIN Yuhong,LI Qingsong,SONG Yali,HUANG Yiming,MA Xiaoyan.Oxidation Degradation and Kinetic Analysis of Emerging Organic Contaminant Saccharin in Water[J].Advanced Engineering Sciences,2022,54(5):210-217.
引用文本:
项硕,金雨鸿,李青松,宋亚丽,黄奕鸣,马晓雁.水中新型有机污染糖精的氧化降解及动力学分析[J].工程科学与技术,2022,54(5):210-217.
XIANG Shuo,JIN Yuhong,LI Qingsong,SONG Yali,HUANG Yiming,MA Xiaoyan.Oxidation Degradation and Kinetic Analysis of Emerging Organic Contaminant Saccharin in Water[J].Advanced Engineering Sciences,2022,54(5):210-217.