UV/H2O2降解水中磺胺嘧啶影响因素及机理

苟玺莹; 张盼月; 钱锋; 王培良; 赵春晓; 宋永会

doi:10.12030/j.cjee.201704031

UV/H2O2降解水中磺胺嘧啶影响因素及机理

1.
湖南大学环境科学与工程学院, 长沙 410082
2.
中国环境科学研究院城市水环境科技创新基地, 北京 100012
3.
环境生物与控制教育部重点实验室(湖南大学), 长沙 410082
基金项目:
国家水体污染控制与治理科技重大专项（2012ZX07202-005）
中图分类号: X703

Influencing factors and mechanism of sulfadiazine degradation by UV/H2O2

1.
College of Environmental Science and Engineering, Hunan University, Changsha 410082, China
2.
Department of Urban Water Environmental Research, Chinese Research Academy of Environmental Sciences, Beijing 100012, China
3.
Key Laboratory of Environmental Biology and Pollution Control(Hunan University), Ministry of Education, Changsha 410082, China
Fund Project:

摘要: 利用UV/H2O2光氧化反应器降解水中的磺胺嘧啶，考察了H2O2投量、pH值、紫外功率等因素对去除效果的影响，同时对反应动力学及降解产物进行了分析。结果表明，在紫外辐照与H2O2氧化共同作用下，UV/H2O2降解水中磺胺嘧啶效果显著，去除率达90%以上，其降解过程符合一级反应动力学模型（R2=0.991 2）。H2O2投量与磺胺嘧啶降解速率常数具有良好的线性关系，H2O2投量由0.03增大至1.50 mmol·L-1，反应速率常数由0.048 2增大至0.359 9 min-1；同时，随着紫外灯功率由5增大至15 W，反应速率常数由0.066 2增大至0.163 1 min-1；随着初始磺胺嘧啶浓度由0.02增加至0.08 mmol·L-1，反应速率常数由0.251 7逐渐降低至0.046 8 min-1；pH由3.0升高至7.0，反应速率常数由0.070 2增大至0.102 3 min-1，当pH继续增大时，反应速率常数反而降低。根据液相色谱/质谱（LC/MS）对中间产物分析，UV/H2O2降解磺胺嘧啶生成质荷比（m/z）为173、186和200的对氨基苯磺酸等中间产物，推测S-N键和C-N键被打开，这些中间产物可进一步被降解，但TOC去除率仅为7%，表明磺胺嘧啶仅部分被矿化。UV/H2O2工艺处理磺胺嘧啶的电能效率（EEO）采用每一对数减少级电能输入进行评价，优化条件下电能效率为0.078 kWh·m-3，可为实际工程应用提供参考。
- 磺胺嘧啶 /
- UV/H2O2 /
- 降解速率常数 /
- 降解产物
Abstract: The UV/H2O2 photo-oxidation reactor was applied to degrade sulfadiazine solution. The effect of H2O2 concentration, initial pH value, UV light power and sulfadiazine concentration on removal efficiency were investigated. The reaction kinetics and degradation products were also analyzed to full understand the degradation process. The results showed that the UV/H2O2 process was effective for the degradation of sulfadiazine with a removal efficiency above 90%, and the degradation process fitted well with the first-order kinetics model (R2=0.991 2). There had a satisfied linear relation between the degradation rate and H2O2 dosage. The degradation rate increased from 0.048 2 to 0.359 9 min-1 when the H2O2 dosage increased from 0.03 to 1.50 mmol·L-1. The degradation rate also increased from 0.066 2 to 0.163 1 min-1 with an increase of UV light power from 5 to 15 W. In contrast, the degradation rate decreased from 0.251 7 to 0.046 8 min-1 with an increase of sulfadiazine concentration from 0.02 to 0.08 mmol·L-1. The pH value also can affect the degradation rate, which increased from 0.070 2 to 0.102 3 min-1 when pH value increased from 3.0 to 7.0. However, the degradation rate decreased to 0.050 2 min-1 when pH value increased to 11.0. The results of liquid chromatography-mass spectrometry (LC/MS) suggested that three intermediate degradation-products were formed with a mass-to-charge ratio (m/z) of 173, 186 and 200, respectively. It was indicated that S-N bonds and N-N bonds were broken in the process, and the intermediate products can further degraded. However, the results showed that only 7% of TOC was removed, indicating that only small part of sulfadiazine were mineralized. Finally, the electrical energy per order (EEO) was used to evaluate the cost of sulfadiazine degradation process in UV/H2O2 photo-oxidation reactor. The results showed that the EEO was only 0.078 kWh·m-3 at the optimum conditions, which can provide a reference for practical engineering application.
- sulfadiazine /
- UV/H2O2 /
- degradation rate constant /
- degradation product

[1]	冯欣欣,杜尔登,郭迎庆,等. UV/H₂O₂降解羟苯甲酮反应动力学及影响因素[J]. 环境科学,2015,36(6):2129-2137
[2]	鲍晓磊,强志民,贲伟伟,等. 磁性纳米复合材料CoFeM48对水中磺胺类抗生素的吸附去除研究[J]. 环境科学学报,2013,33(2):401-407
[3]	BIALK-BIELINSKA A,STOLTE S,ARNING J,et al. Ecotoxicity evaluation of selected sulfonamides[J]. Chemosphere,2011,85(6):928-933
[4]	BARAN W,ADAMEK E,ZIEMIANSKA J,et al. Effects of the presence of sulfonamides in the environment and their influence on human health[J]. Journal of Hazardous Materials,2011,196(1):1-15
[5]	FUKAHORI S,FUJIWARA T. Photocatalytic decomposition behavior and reaction pathway of sulfamethazine antibiotic using TiO₂[J]. Journal of Environmental Management,2015,157:103-110
[6]	JI Y,DONG C,KONG D,et al. Heat-activated persulfate oxidation of atrazine:Implications for remediation of groundwater contaminated by herbicides[J]. Chemical Engineering Journal,2015,263:45-54
[7]	TROVÓ A G,NOGUEIRA R F P,AGVERA A,et al. Paracetamol degradation intermediates and toxicity during photo-Fenton treatment using different iron species[J]. Water Research,2012,46(16):5374-5380
[8]	李青松,高乃云,马晓雁,等. UV/H₂O₂工艺降解水中17α-乙炔基雌二醇[J]. 中国环境科学,2006,26(5):515-518
[9]	KIM I,YAMASHITA N,TANAKA H. Performance of UV and UV/H₂O₂ processes for the removal of pharmaceuticals detected in secondary effluent of a sewage treatment plant in Japan[J]. Journal of Hazardous Materials,2009,166(2/3):1134-1140
[10]	LIAO Q,JI F,LI J C,et al. Decomposition and mineralization of sulfaquinoxaline sodium during UV/H₂O₂ oxidation processes[J]. Chemical Engineering Journal,2016,284:494-502
[11]	ZHANG R C,YANG Y K,HUANG C H,et al. Kinetics and modeling of sulfonamide antibiotic degradation in wastewater and human urine by UV/H₂O₂ and UV/PDS[J]. Water Research,2016,103:283-292
[12]	GARCÍA-GALÁN M J,ANFRUNS A,GONZALEZ-OLMOS R,et al. Advanced oxidation of the antibiotic sulfapyridine by UV/H₂O₂:Characterization of its transformation products and ecotoxicological implications[J]. Chemosphere,2016,147:451-459
[13]	魏红,杨小雨, 李克斌,等. UVA紫外辐射下UV/H₂O₂/KI降解水中磺胺嘧啶[J]. 环境科学学报,2016,36(5):1697-1703
[14]	ZOU X,ZHOU T,MAO J,et al. Synergistic degradation of antibiotic sulfadiazine in a heterogeneous ultrasound-enhanced Fe⁰/persulfate Fenton-like system[J]. Chemical Engineering Journal,2014,257(6):36-44
[15]	BEHNAJADY M A,VAHID B,MODIRSHAHLA N,et al. Evaluation of electrical energy per order (EEO) with kinetic modeling on the removal of malachite green by US/UV/H₂O₂ process[J]. Desalination,2009,249(1):99-103
[16]	BELTRAN F J,OVEJERO G,GARCIAARAYA J F,et al. Oxidation of polynuclear aromatic hydrocarbons in water.2.UV radiation and ozonation in the presence of UV radiation[J]. Industrial & Engineering Chemistry Research,1995,34(5):1607-1615
[17]	FANG J Y,LING L,SHANG C. Kinetics and mechanisms of pH-dependent degradation of halonitromethanes by UV photolysis[J]. Water Research,2013,47(3):1257-1266
[18]	XIAO Y J,ZHANG L F,YUE J Q,et al. Kinetic modeling and energy efficiency of UV/H₂O₂ treatment of iodinated trihalomethanes[J]. Water Research,2015,75:259-269
[19]	GONG P,YUAN H X,ZHAI P P,et al.Investigation on the degradation of benzophenone-3 by UV/H₂O₂ in aqueous solution[J]. Chemical Engineering Journal,2015,277:97-103
[20]	汪力,高乃云,魏宏斌,等. 饮用水中内分泌干扰物阿特拉津UV光氧化研究[J].环境科学,2006,27(6):1144-1149
[21]	张薛,赵璇. UV/H₂O₂氧化处理水中去污剂[J]. 环境科学学报,2015,35(3):750-755
[22]	CHRISTENSEN H,SEHESTED K,CORFITZEN H. Reactions of hydroxyl radicals with hydrogen peroxide at ambient and elevated temperatures[J]. Journal of Physical Chemistry,1982,86(8):1588-1590
[23]	BUXTON G V,GREENSTOCK C L,HELMAN W P,et al. Critical review of rate constants for reactions of hydrated electrons,hydrogen atoms and hydroxyl radicals (·OH/·O^-) in aqueous solution[J]. Journal of Physical & Chemical Reference Data,1988,17(2):513-886
[24]	KIM I Y,KIM M K,YOON Y,et al. Kinetics and degradation mechanism of clofibric acid and diclofenac in UV photolysis and UV/H₂O₂ reaction[J]. Desalination and Water Treatment,2014,52(31/32/33):6211-6218
[25]	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
[26]	AHMED M M,BARBATI S,DOUMENQ P,et al. Sulfate radical anion oxidation of diclofenac and sulfamethoxazole for water decontamination[J]. Chemical Engineering Journal,2012,197(14):440-447

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UV/H2O2降解水中磺胺嘧啶影响因素及机理

Influencing factors and mechanism of sulfadiazine degradation by UV/H2O2

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UV/H2O2降解水中磺胺嘧啶影响因素及机理

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Influencing factors and mechanism of sulfadiazine degradation by UV/H2O2

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UV/H2O2降解水中磺胺嘧啶影响因素及机理

Influencing factors and mechanism of sulfadiazine degradation by UV/H2O2

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UV/H2O2降解水中磺胺嘧啶影响因素及机理

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Influencing factors and mechanism of sulfadiazine degradation by UV/H2O2

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