臭氧氧化降解水中磺胺嘧啶的机理研究

王培良; 钱锋; 宋永会; 苟玺莹

doi:10.3969/j.issn.1674-991X.2017.04.061

臭氧氧化降解水中磺胺嘧啶的机理研究

doi: 10.3969/j.issn.1674-991X.2017.04.061

王培良^1,2,
钱锋¹,
宋永会^1,*, ,,
苟玺莹¹

^1. 中国环境科学研究院城市水环境科技创新基地,北京 100012
^2. 中国地质大学(北京)水资源与环境学院,北京 100083

详细信息

作者简介:
王培良(1991—),男,硕士研究生,研究方向为工业废水处理,wplsunboy320@126.com

通讯作者:
宋永会 E-mail: songyh@craes.org.cn

中图分类号: X703
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出版历程
- 收稿日期: 2016-12-15
- 刊出日期: 2017-07-20

Degradation mechanisms of sulfadiazine in aqueous solution by ozonation

^1. Department of Urban Water Environmental Research, Chinese Research Academy of Environmental Sciences, Beijing 100012, China
^2. School of Water Resources and Environment, Chinese University of Geosciences, Beijing 100083, China

More Information

Corresponding author: Yonghui SONG E-mail: songyh@craes.org.cn

摘要

摘要: 环境中残留的抗生素药物对生态环境的危害受到极大关注。研究了臭氧对水中磺胺嘧啶(SD)的降解,考察了溶液pH、臭氧浓度和HC $O 3 -$ 投加量对臭氧降解SD的影响,并对其降解机理进行了分析。结果表明:初始pH、臭氧浓度及HC $O 3 -$ 均对臭氧氧化降解SD过程造成影响,提高pH、增加臭氧浓度和HC $O 3 -$ 投加量均能提高SD降解速率;在SD浓度为30 mg/L、初始pH为9.14、臭氧浓度为10.0 mg/L、HC $O 3 -$ 投加量为100 mg/L时,反应30 min后SD基本被去除,120 min后SD的最终矿化率为39.44%;臭氧降解SD过程基本符合伪一级动力学模型。液相色谱-质谱分析结果显示:臭氧氧化SD过程中,生成中间产物对氨基苯磺酸(C₆H₇NO₃S),经臭氧进一步氧化分解,最终矿化生成CO₂。
- 磺胺嘧啶 /
- 臭氧氧化 /
- 动力学 /
- 降解产物
Abstract: The harm of antibiotics in the environment is of great concern to the ecological environment. The degradation of sulfadiazine (SD) by ozone was studied. The effects of pH, ozone concentration and HC $O 3 -$ concentration on the degradation of SD were investigated, and the degradation mechanisms were also analyzed. The results showed that the initial pH, the ozone concentration and HC $O 3 -$ all had effects on the SD degradation process, and the initial pH, the ozone concentration and HC $O 3 -$ concentration could increase the degradation rate of SD. At initial pH of 9.14, SD concentration of 30 mg/L, ozone concentration of 10.0 mg/L and HC $O 3 -$ dosage of 100 mg/L, the SD was primarily removed after a reaction time of 30 min and finally reached a mineralization rate of 39.44% at 120 min. The SD process of ozone degradation was basically in accordance with pseudo-first-order kinetics model. The results of liquid chromatography-mass spectrometry showed that, in the course of ozone oxidation, the formation of p-aminobenzenesulfonic acid (C₆H₇NO₃S) was produced and being further oxidized by ozone and finally mineralized to form CO₂.
- sulfadiazine /
- ozone oxidation /
- kinetics /
- degradation products

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参考文献(31)

[1]	孙丰霞 . 污水处理系统中磺胺嘧啶和磺胺甲❚唑的优化处理研究 [D]. 泰安:山东农业大学, 2014.
[2]	周宁娟, 薛罡, 卜聃 , 等. 羟基化锌催化臭氧氧化去除水中痕量磺胺嘧啶[J]. 中国环境科学, 2011,31(2):233-238. ZHOU N J, XUE G, BU D , et al. Catalytic ozonation of trace sulfadiazine in water by ZnOOH[J]. China Environmental Science, 2011,31(2):233-238.
[3]	张佳 . 电催化氧化降解磺胺嘧啶模拟废水的研究[D]. 南京:南京师范大学, 2014.
[4]	MATAMOROS V, BAYONA J M . Elimination of pharmaceuticals and personal care products in subsurface flow constructed wetlands[J]. Environmental Science and Technology, 2006,40(18):5811-5816.
[5]	崔晓宇, 何绪文, 曾萍 , 等. UASB-MBR组合工艺处理黄连素废水的中试[J]. 环境科学研究, 2015,28(8):1295-1301. CUI X Y, HE X W, ZENG P , et al. A pilot-scale hybrid upflow anaerobic sludge blanket reactor (UASB)-membrane bioreactor (MBR) system for berberine wastewater treatment[J]. Research of Environmental Sciences, 2015,28(8):1295-1301.
[6]	BUSER H R, BALMER M E, SCHMID P , et al. Occurrence of UV filters 4-methylbenzylidene camphor and octocrylene in fish from various Swiss rivers with inputs from wastewater treatment plants[J]. Environmental Science and Technology, 2006,40(5):1427-1431.
[7]	ADAMS C, ASCE M, WANG Y , et al. Removal of antibiotics from surface and distilled water in conventional water treatment processes[J]. Journal of Environmental Engineering, 2002,128(3):253-260.
[8]	NAKADA N, SHINOHARA H, MURATA A , et al. Removal of selected pharmaceuticals and personal care products (PPCPs) and endocrine-disrupting chemicals (EDCs) during sand filtration and ozonation at a municipal sewage treatment plant[J]. Water Research, 2007,41(19):4373-4382.
[9]	曾萍, 宋永会 , DRESELY J, 等. 金刚烷胺模拟废水Fenton氧化及其中间产物分析[J]. 环境工程技术学报, 2011,1(6):455-459. ZENG P, SONG Y H, DRESELY J , et al. Oxidative degradation of simulated amantadine by the Fenton processes and the intermediates analysis[J]. Journal of Environmental Engineering Technology, 2011,1(6):455-459.
[10]	JAVIER B F, ACERO J L, REAL F J , et al. Ozonation of pharmaceutical compounds: rate constants and elimination in various water matrices[J]. Chemosphere, 2009,77(1):53-59.
[11]	ANDREOZZI R, CAPRIO V, MAROTTA R , et al. Paracetamol oxidation from aqueous solutions by means of ozonation and H₂O₂ /UV system[J]. Water Research, 2003,37(5):993-1004.
[12]	李魁, 林齐, 宋永会 , 等. 制药园区难降解尾水强化预处理试验研究[J]. 环境工程技术学报, 2014,4(5):373-377. LI K, LIN Q, SONG Y H , et al. Study on intensive pretreatment of refractory pharmaceutical park tail water[J]. Journal of Environmental Engineering Technology, 2014,4(5):373-377.
[13]	YANG L, YU L, RAY M B . Degradation of paracetamol in aqueous solutions by TiO₂ photocatalysis[J]. Water Research, 2008,42(13):3480-3488.
[14]	秦伟伟, 肖书虎, 宋永会 , 等. O₃/UV协同氧化处理黄连素制药废水[J]. 环境科学研究, 2010,23(7):877-881. QIN W W, XIAO S H, SONG Y H , et al. Treatment of berberine pharmaceutical wastewater by O3/UV synergetic oxidation[J]. Research of Environmental Sciences, 2010,23(7):877-881.
[15]	杨岸明, 常江, 甘一萍 , 等. 臭氧氧化二级出水有机物可生化性研究[J]. 环境科学, 2010,31(2):363-367. YANG A M, CHANG J, GAN Y P , et al. Research on the organic biodegradability of secondary effluent treated by ozonation[J]. Environmental Science, 2010,31(2):363-367.
[16]	徐新华, 赵伟荣 . 水和废水的臭氧处理[M], 北京: 化学工业出版社, 2003.
[17]	张彭义, 祝万鹏 . 臭氧水处理技术的进展[J]. 环境科学进展, 1995(6):18-24.
[18]	HONG P K, ZENG Y . Degradation of pentachlorophenol by ozonation and biodegradability of intermediates[J]. Water Research, 2002,36(17):4243-4254.
[19]	徐武军, 张国臣, 郑明霞 , 等. 臭氧氧化技术处理含抗生素废水[J]. 化学进展, 2010(5):1002-1009. XU W J, ZHANG G C, ZHENG M X , et al. Treatment of antibiotic wastewater by ozonation[J]. Progress in Chemistry, 2010(5):1002-1009.
[20]	邱光磊, 宋永会, 曾萍 , 等. UASB-MBR组合工艺处理模拟黄连素废水[J]. 环境科学研究, 2010,23(7):942-947. QIU G L, SONG Y H, ZENG P , et al. Treatment of synthetic berberine wastewater in a hybrid upflow anaerobic sludge blanket reactor (UASB)-membrane bioreactor (MBR) system[J]. Research of Environmental Sciences, 2010,23(7):942-947.
[21]	ANDREOZZI R, CANTERINO M, MAROTTA R , et al. Antibiotic removal from wastewaters: the ozonation of amoxicillin[J]. Journal of Hazardous Materials, 2005,122(3):243-250.
[22]	KU Y, SU A W, SHEN Y S . Decomposition kinetics of ozone in aqueous solution[J]. Industrial and Engineering Chemistry Research, 1996,35(10):3369-3374.
[23]	张可佳, 殷娣娣, 高乃云 , 等. 水中两种微囊藻毒素的臭氧氧化及其影响因素[J]. 中国环境科学, 2008,28(10):877-882. ZHANG K J, YIN D D, GAO N Y , et al. Effect and influence of two representative microcystins degradation by ozonation in water[J]. China Environmental Science, 2008,28(10):877-882.
[24]	CATORCENO L L C, NOGUEIRA K R B, TEIXEIRA A C S C . Treatment of aqueous effluents containing phenol by the O₃,O₃-UV,and O₃-H₂O₂ processes: experimental study and neural network modeling[J]. Separation Science and Technology, 2010,45(11):1521-1528.
[25]	吴南村, 尹平河, 赵玲 , 等. 水体中微污染磺胺嘧啶药物的氧化降解[J]. 生态环境, 2008(6):2183-2186.
[26]	李明亮 . 环境中磺胺类药物的降解行为及影响因素的研究[D]. 新乡:河南师范大学, 2012.
[27]	GARCIA-ARAYA J F, BELTRAN F J, AGUINACO A . Diclofenac removal from water by ozone and photolytic TiO₂ catalysed processes[J]. Journal of Chemical Technology and Biotechnology, 2010,85(6):798-804.
[28]	LARSON R A, ZEPP R G . Reactivity of the carbonate radical with aniline derivatives[J]. Environmental Toxicology and Chemistry, 1988,7(7):265-274.
[29]	WESTERHOFF P, YOON Y, SNYDER S , et al. Fate of endocrine-disruptor,pharmaceutical,and personal care product chemicals during simulated drinking water treatment processes[J]. Environmental Science and Technology, 2005,39(17):6649-6663.
[30]	BARAN W, ADAMEK E, SOBCZAK A , et al. The comparison of photocatalytic activity of Fe-salts,TiO₂,and TiO₂/FeCl₃ during the sulfanilamide degradation process[J]. Catalysis Communications, 2009,10(6):811-814.
[31]	潘诗卉 . 磺胺嘧啶在紫外辐射下的降解机理探讨[D]. 上海:上海师范大学, 2014.