环境因子对腐殖酸诱导双氯芬酸光降解的影响
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摘要
采用腐殖酸(HA)作为溶解有机质的代表物,考察了HA浓度、p H、离子强度和溶解氧等环境因子对HA诱导双氯芬酸(DCF)光降解的影响。结果表明:DCF在纯水和HA溶液中的光化学降解过程均服从一级动力学规律。与DCF纯水溶液相比,当HA浓度由0增至5. 0 mg C/L时,DCF光降解速率增大,但当HA浓度高于5. 0 mg C/L时,DCF的光降解过程受到抑制。在环境浓度水平(5. 0 mg C/L)下,HA对DCF光降解的诱导作用随DCF初始浓度增大而逐渐减弱。同时,HA对DCF光降解的诱导作用还受到多种水环境因子的影响,其随p H增大先减弱后增强,随离子强度增大而增强,随溶解氧浓度增大而减弱。研究结果可为环境水体中药物的归趋预测及生态风险评价提供依据。
Humic acid( HA) was selected as a representative compound for dissolved organic matter and influences of HA concentration,p H,ionic strength and dissolved oxygen on the HA-induced photodegradation of diclofenac( DCF) were studied. The results showed that the degradation of DCF obeyed the first-order kinetics model in either pure water or HA solutions. Compared to DCF in pure water,the photodegradation rate of DCF in HA solutions increased as increasing of the HA concentration in the range of from 0 to5. 0 mg C/L,while decreased as increasing of the HA concentration when higher than 5. 0 mg C/L. At the environmentally relevant concentration level( 5. 0 mg C/L),the promotion effect of HA was weakened by higher initial concentrations of DCF. The promotion effect of HA was also closely related to water matrix properties,for example,it was initially weakened and then strengthened as the p H increased,it was strengthened as the ionic strength increased but was weakened as the dissolved oxygen concentration increased. The results of this study provided supports on the fate prediction and ecological risk assessment of pharmaceuticals in the aquatic environment.
Humic acid( HA) was selected as a representative compound for dissolved organic matter and influences of HA concentration,p H,ionic strength and dissolved oxygen on the HA-induced photodegradation of diclofenac( DCF) were studied. The results showed that the degradation of DCF obeyed the first-order kinetics model in either pure water or HA solutions. Compared to DCF in pure water,the photodegradation rate of DCF in HA solutions increased as increasing of the HA concentration in the range of from 0 to5. 0 mg C/L,while decreased as increasing of the HA concentration when higher than 5. 0 mg C/L. At the environmentally relevant concentration level( 5. 0 mg C/L),the promotion effect of HA was weakened by higher initial concentrations of DCF. The promotion effect of HA was also closely related to water matrix properties,for example,it was initially weakened and then strengthened as the p H increased,it was strengthened as the ionic strength increased but was weakened as the dissolved oxygen concentration increased. The results of this study provided supports on the fate prediction and ecological risk assessment of pharmaceuticals in the aquatic environment.
引文
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[3]Boxall A B A,Rudd M A,Brooks B W,et al.Pharmaceuticals and personal care products in the environment:What are the big questions[J].Environmental Health Perspectives,2012,120(9):1221-1229.
[4]Martínez C,Fernández M I,Santaballa J A,et al.Aqueous degradation of diclofenac by heterogeneous photocatalysis using nanostructured materials[J].Applied Catalysis B:Environmental,2011,107(1-2):110-118.
[5]Zhang Y,Geien S U,Gal C.Carbamazepine and diclofenac:Removal in wastewater treatment plants and occurrence in water bodies[J].Chemosphere,2008,73(8):1151-1161.
[6]Wang Y,Liu H,Liu G,et al.Kinetics for diclofenac degradation by chlorine dioxide in aqueous media:Influences of natural organic matter additives[J].Journal of the Taiwan Institute of Chemical Engineers,2015,56:131-137.
[7]Kallio J M,Lahti M,Oikari A,et al.Metabolites of the aquatic pollutant diclofenac in fish bile[J].Environmental Science&Technology,2010,44(19):7213-7219.
[8]Poirier-Larabie S,Segura P A,Gagnon C.Degradation of the pharmaceuticals diclofenac and sulfamethoxazole and their transformation products under controlled environmental conditions[J].Science of the Total Environment,2016,557:257-267.
[9]张楠,刘国光,刘海津,等.双氯芬酸在水环境中光降解的初步研究[J].环境化学,2013,32(1):42-47.
[10]Chianese S,Iovino P,Leone V,et al.Photodegradation of diclofenac sodium salt in water solution:Effect of HA,NO3-and Ti O2on photolysis performance[J].Water,Air,&Soil Pollution,2017,228(8):270.
[11]Zhang N,Liu G,Liu H,et al.Diclofenac photodegradation under simulated sunlight:Effect of different forms of nitrogen and kinetics[J].Journal of Hazardous Materials,2011,192(1):411-418.
[12]Zhang N,Li J M,Liu G G,et al.Photodegradation of diclofenac in aqueous solution by simulated sunlight irradiation:Kinetics,thermodynamics and pathways[J].Water Science&Technology,2017,75(9-10):2163-2171.
[13]Zhang N,Liu H J,Liu G G,et al.Role of cetyltrimethyl ammonium bromide,crystal violet and humic acid in the degradation of diclofenac under simulated sunlight irradiation[J].Science China Chemistry,2012,55(12):2610-2616.
[14]任东,杨小霞,马晓冬,等.DOM结构特征及其对17β-雌二醇光降解的影响[J].中国环境科学,2015,35(5):1375-1383.
[15]Chen Y,Zhang K,Zuo Y.Direct and indirect photodegradation of estriol in the presence of humic acid,nitrate and iron complexes in water solutions[J].Science of the Total Environment,2013,463:802-809.
[16]Parker K M,Pignatello J J,Mitch W A.Influence of ionic strength on triplet-state natural organic matter loss by energy transfer and electron transfer pathways[J].Environmental Science&Technology,2013,47(19):10987-10994.
[17]Chen C,Wang X,Jiang H,et al.Direct observation of macromolecular structures of humic acid by AFM and SEM[J].Colloids and Surfaces A:Physicochemical and Engineering Aspects,2007,302(1):121-125.
[18]Zhang N,Li J M,Liu G G,et al.Photodegradation of diclofenac in seawater by simulated sunlight irradiation:The comprehensive effect of nitrate,Fe(III)and chloride[J].Marine Pollution Bulletin,2017,117(1-2):386-391.
[19]Koumaki E,Mamais D,Noutsopoulos C,et al.Degradation of emerging contaminants from water under natural sunlight:The effect of season,pH,humic acids and nitrate and identification of photodegradation by-products[J].Chemosphere,2015,138:675-681.
[20]白泽琳,何伟,李一龙,等.光诱导腐殖酸产生单线态氧的影响因素研究[J].环境科学学报,2016,36(4):1169-1175.