Ag/g-C3N4可见光催化技术降解水中磺胺嘧啶的研究
Study on degradation of sulfadiazine in water by visible-light catalytic technology of Ag/g-C3N4
-
摘要: 将Ag/g-C3N4(银/石墨相氮化碳)可见光催化技术应用于废水中磺胺嘧啶的去除,考察Ag/g-C3N4对磺胺嘧啶的降解效果、水质因素对降解效果的影响、降解机理、中间产物及其应用于实际水体时磺胺嘧啶的降解情况.结果表明:1)质量分数为5%的Ag/g-C3N4在可见光照射下能将磺胺嘧啶有效降解,去除率高达98.3%,且降解过程符合拟一级动力学模型;2)溶液的pH值和碱度对Ag/g-C3N4降解磺胺嘧啶的效果影响不大,但溶液中腐殖酸的存在对磺胺嘧啶的降解起抑制作用;3)在磺胺嘧啶的降解过程中,·O2-和光生空穴是主要的活性物种;4)降解过程主要产生4种中间产物,分别为2-氨基嘧啶、对氨基苯磺酸、羟基化磺胺嘧啶和硝基化磺胺嘧啶;5)以松花江水和生活污水的二级出水为水质背景时,Ag/g-C3N4对磺胺嘧啶的去除率分别为95.4%和77.5%.Abstract: Visible-light catalysis technology of Ag/g-C3N4 (silver/graphite carbon nitride) was applied to the removal of sulfadiazine in wastewater. The degradation effect of Ag/g-C3N4 on sulfadiazine and water quality factors,degradation mechanism,intermediate products and its degradation effect on sulfadiazine in actual water were investigated. The results showed that Ag/g-C3N4 with a mass fraction of 5% could effectively degrade sulfadiazine under visible-light irradiation,with a removal rate of up to 98.3%,and the degradation process conformed to the pseudo-first-order kinetic model; the pH and alkalinity of the solution Ag/g-C3N4 had little effect on the degradation of sulfadiazine,but the presence of humic acid in the solution inhibited the degradation of sulfadiazine; during the degradation of sulfadiazine,·O2- and photogenerated holes were the main activities species; the degradation process mainly produced 4 kinds of intermediate products,which were 2-aminopyrimidine,p-aminobenzenesulfonic acid,hydroxylated sulfadiazine,and nitrated sulfadiazine. When the Songhua River water and the secondary effluent of domestic sewage were used as the water quality background,the removal rates of Ag/g-C3N4 for sulfadiazine were 95.4% and 77.5%,respectively.
-
Key words:
- Ag/g-C3N4 /
- visible-light catalytic technology /
- sulfadiazine /
- degradation mechanism
-
-
[1]
苟玺莹,张盼月,钱锋,等.UV/H2O2降解水中磺胺嘧啶影响因素及机理[J].环境工程学报,2017,11(11):5810.
-
[2]
KVMMERER K.Antibiotics in the aquatic environment-a review-part Ⅱ[J].Chemosphere,2009,75(4):435.
-
[3]
BU Q,WANG B,HUANG J,et al.Pharmaceuticals and personal care products in the aquatic environment in China:a review[J] Journal of Hazardous Materials,2013,262:189.
-
[4]
ZHANG T,LI B.Occurrence,transformation,and fate of antibiotics in municipal wastewater treatment plants[J].Critical Reviews in Environmental Science and Technology,2011,41:951.
-
[5]
王国庆,刘云,柯玮,等.超高效液相色谱-静电场轨道离子阱高分辨质谱联用筛查分析饲料中抗菌类药物[J].轻工学报,2016,31(4):15.
-
[6]
CLARA M,STRENN B,GANS O,et al.Removal of selected pharmaceuticals,fragrances and endocrine disrupting compounds in a membrane bioreactor and conventional wastewater treatment plants[J].Water Research,2005,39(19):4797.
-
[7]
DEWIL R,MANTZAVINOS D,POULIOS I,et al.New perspectives for advanced oxidation processes[J].Journal of Environmental Management,2017,195:93.
-
[8]
AO X,LIU W.Degradation of sulfamethoxazole by medium pressure UV and oxidants:Peroxymonosulfate,persulfate,and hydrogen peroxide[J].Chemical Engineering Journal,2017,313:629.
-
[9]
魏红,杨小雨,李克斌,等.UVA紫外辐射下H2O2/KI降解水中磺胺嘧啶[J].环境科学学报,2016,36(5):1697.
-
[10]
IOANNIDOU E,FRONTISTIS Z,ANTONOPOULOU M,et al.Solar photocatalytic degradation of sulfamethoxazole over tungsten modified TiO2[J].Chemical Engineering Journal,2017,318:143.
-
[11]
邵鹏辉.纳米氧化铁的优化制备及其可见光芬顿降解水中的双酚S[D].哈尔滨:哈尔滨工业大学,2017.
-
[12]
SONG Y,QI J,TIAN J,et al.Construction of Ag/g-C3N4 photocatalysts with visible-light photocatalytic activity for sulfamethoxazole degradation[J].Chemical Engineering Journal,2018,341:547.
-
[13]
BAI X,WANG L,WANG Y,et al.Enhanced oxidation ability of g-C3N4 photocatalyst via C60 modification[J].Applied Catalysis B:Environmental,2014(152/153):262.
-
[14]
宋亚丽,张光明,常爱敏,等.US/Zn0体系降解水中的对硝基苯甲酸[J].环境工程学报, 2014,8(5):1797.
-
[15]
WANG J,YANG Z,GAO X,et al.Core-shell g-C3N4@ZnO composites as photoanodes with double synergistic effects for enhanced visible-light photoelectrocatalytic activities[J].Applied Catalysis B:Environmental,2017,217:169.
-
[16]
宋亚丽.g-C3N4基可见光催化剂降解水中典型磺胺类抗生素的研究[D].哈尔滨:哈尔滨工业大学,2018.
-
[17]
CUI Y,DING Z,LIU P,et al.Metal-free activation of H2O2 by g-C3N4 under visible light irradiation for the degradation of organic pollutants[J].Physical Chemistry Chemical Physics,2012,14(4):1455.
-
[18]
YANG Y,LU X,JIANG J,et al.Degradation of sulfamethoxazole by UV,UV/H2O2 and UV/persulfate (PDS):Formation of oxidation products and effect of bicarbonate[J].Water Research,2017,118:196.
-
[19]
江进.高价态锰、铁氧化降解水中典型有机物的特性与机理研究[D].哈尔滨:哈尔滨工业大学,2009.
-
[20]
CHAN K,CHU W.Effect of humic acid on the photolysis of the pesticide atrazine in a surfactant-aided soil-washing system in acidic condition[J].Water Research,2005,39(10),2154.
-
[1]
计量
- PDF下载量: 6
- 文章访问数: 1168
- 引证文献数: 0