水体中布洛芬的间接光降解作用机理研究
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摘要
为阐明布洛芬(IBP)在海水中的间接光降解机理,研究了4种不同来源的溶解有机物(DOM)以及溶液初始pH值、盐度、NO3-和HCO3-对IBP间接光降解的影响.结果表明,4种DOM均可促进IBP的间接光降解作用,降解过程符合准一级反应动力学, 4种DOM对IBP间接光降解的促进效果从大到小为:腐殖酸(JKHA)>Suwannee河腐殖酸(SRHA)>Suwannee河富里酸(SRFA)>Suwannee河天然有机物(SRNOM).DOM主要通过产生活性自由基促进IBP的间接光降解过程,其中1O2和·OH的作用较显著.在初始p H5～11的范围内,IBP的光降解速率先降低后增加,在p H5时最快.盐度、NO3-和HCO3-初始浓度的增加均会促进IBP的间接光降解.
To clarify the indirect photodegradation mechanism of IBP, the indirect photodegradation behaviors of IBP were investigated in the presence of four kinds of dissolved organic matter(DOM) and were also assessed in the presence of seawater components and conditions such as salinity, p H, nitrate and bicarbonate. Firstly, the indirect photodegradation of IBP could be accelerated by the four different sources of DOM and followed pseudo-first-order kinetics, the photodegradation rate constants of APAP were found to decrease in the following order: JKHA> SRHA> SRFA> SRNOM. DOM promoted the indirect photodegradation of IBP through the formation of various reactive intermediates, ·OH and 1 O2 were the main contributors. Secondly, in the range of pH 5～11, the photodegradation rate of IBP was firstly decreased and then increased, the highest photodegradation rate of IBP was found at pH 5.0. Lastly, the photodegradation rate constants of IBP increased with increasing salinity, nitrate and bicarbonate.
To clarify the indirect photodegradation mechanism of IBP, the indirect photodegradation behaviors of IBP were investigated in the presence of four kinds of dissolved organic matter(DOM) and were also assessed in the presence of seawater components and conditions such as salinity, p H, nitrate and bicarbonate. Firstly, the indirect photodegradation of IBP could be accelerated by the four different sources of DOM and followed pseudo-first-order kinetics, the photodegradation rate constants of APAP were found to decrease in the following order: JKHA> SRHA> SRFA> SRNOM. DOM promoted the indirect photodegradation of IBP through the formation of various reactive intermediates, ·OH and 1 O2 were the main contributors. Secondly, in the range of pH 5～11, the photodegradation rate of IBP was firstly decreased and then increased, the highest photodegradation rate of IBP was found at pH 5.0. Lastly, the photodegradation rate constants of IBP increased with increasing salinity, nitrate and bicarbonate.
引文
[1]Benotti M,Brownawell B.Microbial degradation of pharmaceuticals in estuarine and coastal seawater[J].Environmental Pollution,2009,157(3):994-1002.
[2]Carballa M,Omil F,Lema J M,et al.Behavior of pharmaceuticals,cosmetics and hormones in a sewage treatment plant[J].Water Research,2004,38(12):2918-2926.
[3]Snyder S A,Westerhoff P,Yoon Y,et al.Pharmaceuticals,Personal Care Products,and Endocrine Disruptors in Water:Implications for the Water Industry[J].Environmental Engineering Science,2004,20(5):449-469.
[4]Daughton C G,Ternes T A.Pharmaceuticals and personal care products in the environment:agents of subtle change[J].Environmental Health Perspectives,1999,107(6):907-938.
[5]Scheytt T,Mersmann P,Lindst?dt R,et al.1-octanol/water partition coefficients of 5pharmaceuticals from human medical care:carbamazepine,clofibric acid,diclofenac,ibuprofen,and propyphenazone[J].Water,Air,and Soil Pollution,2005,165(1-4):3-11.
[6]Ghauch A,Tuqan A M,Kibbi N.Ibuprofen removal by heated persulfate in aqueous solution:a kinetics study[J].Chemical Engineering Journal,2012,197:483-492.
[7]Vieno N M,Tuhkanen T,Kronberg L.Seasonal variation in the occurrence of pharmaceuticals in effluents from a sewage treatment plant and in the recipient water[J].Environmental Science and Technology,2005,39(21):8220-8226.
[8]Bahnmüller S,Gunten U V,Canonica S.Sunlight-induced transformation of sulfadiazine and sulfamethoxazole in surface waters and wastewater effluents[J].Water Research,2014,57:183-192.
[9]Jannis W,Urs V G,Silvio C.Effect of Dissolved Organic Matter on the Transformation of Contaminants Induced by Excited Triplet States and the Hydroxyl Radical[J].Environmental Science and Technology,2011,45(4):1334-1340.
[10]Jacobs L E,Fimmen R L,Chin Y P,et al.Fulvic acid mediated photolysis of ibuprofen in water[J].Water Research,2011,45(15):4449-4458.
[11]Li R,Zhao C,Yao B,et al.Photochemical Transformation of Aminoglycoside Antibiotics in Simulated Natural Waters[J].Environmental Science and Technology,2016,50(6):2921-2930.
[12]Xu Y,Nguyen T V,Reinhard M,et al.Photodegradation kinetics of p-tert-octylphenol,4-tert-octylphenoxy-acetic acid and ibuprofen under simulated solar conditions in surface water[J].Chemosphere,2011,85(5):790-796.
[13]Niu X,Liu C,Gutierrez L,et al.Photobleaching-induced changes in photosensitizing properties of dissolved organic matter[J].Water Research,2014,66:140-148.
[14]Bai Y,Cui Z,Su R,et al.Influence of DOM components,salinity,pH,nitrate,and bicarbonate on the indirect photodegradation of acetaminophen in simulated coastal waters[J].Chemosphere,2018,205:108-117.
[15]Oliveira C,Lima D L,Silva C P,et al.Photodegradation of sulfamethoxazole in environmental samples:The role of pH,organic matter and salinity[J].Science of The Total Environment,2019,648:1403-1410.
[16]Batista A P S,Teixeira A C S,Cooper W J,et al.Correlating the chemical and spectroscopic characteristics of natural organic matter with the photodegradation of sulfamerazine[J].Water Research,2016,93:20-29.
[17]Timko S A,Romera-Castillo C,JafféR,et al.Photo-reactivity of natural dissolved organic matter from fresh to marine waters in the Florida Everglades,USA[J].Environmental Science Processes&Impacts,2014,16(4):866-878.
[18]Chen Y,Hu C,Hu X,et al.Indirect photodegradation of amine drugs in aqueous solution under under simulated sunlight[J].Environmental Science and Technology,2009,43(8):2760-2765.
[19]Baena-Nogueras R M,González-Mazo E,Lara-Martín P A.Degradation kinetics of pharmaceuticals and personal care products in surface waters:photolysis vs biodegradation[J].Science of The Total Environment,2017,590:643-654.
[20]Illés E,Takács E,Dombi A,et al.Hydroxyl radical induced degradation of ibuprofen[J].Science of The Total Environment,2013,447:286-292.
[21]Ritchie J D,Perdue E M.Proton-binding study of standard and reference fulvic acids,humic acids,and natural organic matter[J].Geochimica et Cosmochimica Acta,2003,67(1):85-96.
[22]Yamashita Y,Mccallister S L,Koch B P,et al.Dynamics of dissolved organic matter in fjord ecosystems:contributions of terrestrial dissolved organic matter in the deep layer[J].Estuarine,Coastal and Shelf Science,2015,159:37-49.
[23]De Bruyn W J,Clark C D,Ottelle K,et al.Photochemical degradation of phenanthrene as a function of natural water variables modeling freshwater to marine environments[J].Marine pollution bulletin,2012,64(3):532-538.
[24]杨凯,葛林科,那广水,等.水中噁唑烷酮类抗生素利奈唑酮的光化学行为[J].环境通报,2012,57(26):2469-2474.Yang K,Ge L K,Na G S,et al.Aqueous photochemical behavior of oxazolidinone antibiotic linezolid(in Chinese).Chin Sci Bull(Chin Ver),2012,57(26):2469-2474.
[25]Assel M,Laenen R,Laubereau A.Ultrafast electron trapping in an aqueous Na Cl-solution[J].Chemical Physics Letters,1998,289(3-4):267-274.
[26]Mostofa K M G,Sakugawa H.Spatial and temporal variations and factors controlling the concentrations of hydrogen peroxide and organic peroxides in rivers[J].Environmental Chemistry,2009,6(6):524-534.
[27]Brigante M,Minella M,Mailhot G,et al.Formation and reactivity of the dichloride radical(Cl2-)in surface waters:a modelling approach[J].Chemosphere,2014,95:464-469.
[28]Mack J,Bolton J.Photochemistry of nitrite and nitrate in aqueous solution:a review[J].Journal of Photochemistry and Photobiology A:Chemistry,1999,128(1-3):1-13.
[29]Zepp R,HoignéJ,Bader H.Nitrate-induced photooxidation of trace organic chemicals in water[J].Environmental Science and Technology,1987,21(5):443-450.
[30]Espinoza L,Neamtu M.The effect of nitrate,Fe(III)and bicarbonate on the degradation of bisphenol A by simulated solar-UV irradiation[J].Water Research,2007,41(19):4479-4487.
[31]Lin A Y C,Wang X H,Lee W N.Phototransformation determines the fate of 5-fluorouracil and cyclophosphamide in natural surface waters[J].Environmental Science and Technology,2013,47(9):4104-4112.
[32]Vione D,Falletti G,Maurino V,et al.Sources and Sinks of Hydroxyl Radicals upon Irradiation of Natural Water Samples[J].Environmental Science and Technology,2006,40(12):3775-3781.
[33]Wu C,Linden K G.Phototransformation of selected organophosphorus pesticides:roles of hydroxyl and carbonate radicals[J].Water Research,2010,44(12):3585-3594.
[2]Carballa M,Omil F,Lema J M,et al.Behavior of pharmaceuticals,cosmetics and hormones in a sewage treatment plant[J].Water Research,2004,38(12):2918-2926.
[3]Snyder S A,Westerhoff P,Yoon Y,et al.Pharmaceuticals,Personal Care Products,and Endocrine Disruptors in Water:Implications for the Water Industry[J].Environmental Engineering Science,2004,20(5):449-469.
[4]Daughton C G,Ternes T A.Pharmaceuticals and personal care products in the environment:agents of subtle change[J].Environmental Health Perspectives,1999,107(6):907-938.
[5]Scheytt T,Mersmann P,Lindst?dt R,et al.1-octanol/water partition coefficients of 5pharmaceuticals from human medical care:carbamazepine,clofibric acid,diclofenac,ibuprofen,and propyphenazone[J].Water,Air,and Soil Pollution,2005,165(1-4):3-11.
[6]Ghauch A,Tuqan A M,Kibbi N.Ibuprofen removal by heated persulfate in aqueous solution:a kinetics study[J].Chemical Engineering Journal,2012,197:483-492.
[7]Vieno N M,Tuhkanen T,Kronberg L.Seasonal variation in the occurrence of pharmaceuticals in effluents from a sewage treatment plant and in the recipient water[J].Environmental Science and Technology,2005,39(21):8220-8226.
[8]Bahnmüller S,Gunten U V,Canonica S.Sunlight-induced transformation of sulfadiazine and sulfamethoxazole in surface waters and wastewater effluents[J].Water Research,2014,57:183-192.
[9]Jannis W,Urs V G,Silvio C.Effect of Dissolved Organic Matter on the Transformation of Contaminants Induced by Excited Triplet States and the Hydroxyl Radical[J].Environmental Science and Technology,2011,45(4):1334-1340.
[10]Jacobs L E,Fimmen R L,Chin Y P,et al.Fulvic acid mediated photolysis of ibuprofen in water[J].Water Research,2011,45(15):4449-4458.
[11]Li R,Zhao C,Yao B,et al.Photochemical Transformation of Aminoglycoside Antibiotics in Simulated Natural Waters[J].Environmental Science and Technology,2016,50(6):2921-2930.
[12]Xu Y,Nguyen T V,Reinhard M,et al.Photodegradation kinetics of p-tert-octylphenol,4-tert-octylphenoxy-acetic acid and ibuprofen under simulated solar conditions in surface water[J].Chemosphere,2011,85(5):790-796.
[13]Niu X,Liu C,Gutierrez L,et al.Photobleaching-induced changes in photosensitizing properties of dissolved organic matter[J].Water Research,2014,66:140-148.
[14]Bai Y,Cui Z,Su R,et al.Influence of DOM components,salinity,pH,nitrate,and bicarbonate on the indirect photodegradation of acetaminophen in simulated coastal waters[J].Chemosphere,2018,205:108-117.
[15]Oliveira C,Lima D L,Silva C P,et al.Photodegradation of sulfamethoxazole in environmental samples:The role of pH,organic matter and salinity[J].Science of The Total Environment,2019,648:1403-1410.
[16]Batista A P S,Teixeira A C S,Cooper W J,et al.Correlating the chemical and spectroscopic characteristics of natural organic matter with the photodegradation of sulfamerazine[J].Water Research,2016,93:20-29.
[17]Timko S A,Romera-Castillo C,JafféR,et al.Photo-reactivity of natural dissolved organic matter from fresh to marine waters in the Florida Everglades,USA[J].Environmental Science Processes&Impacts,2014,16(4):866-878.
[18]Chen Y,Hu C,Hu X,et al.Indirect photodegradation of amine drugs in aqueous solution under under simulated sunlight[J].Environmental Science and Technology,2009,43(8):2760-2765.
[19]Baena-Nogueras R M,González-Mazo E,Lara-Martín P A.Degradation kinetics of pharmaceuticals and personal care products in surface waters:photolysis vs biodegradation[J].Science of The Total Environment,2017,590:643-654.
[20]Illés E,Takács E,Dombi A,et al.Hydroxyl radical induced degradation of ibuprofen[J].Science of The Total Environment,2013,447:286-292.
[21]Ritchie J D,Perdue E M.Proton-binding study of standard and reference fulvic acids,humic acids,and natural organic matter[J].Geochimica et Cosmochimica Acta,2003,67(1):85-96.
[22]Yamashita Y,Mccallister S L,Koch B P,et al.Dynamics of dissolved organic matter in fjord ecosystems:contributions of terrestrial dissolved organic matter in the deep layer[J].Estuarine,Coastal and Shelf Science,2015,159:37-49.
[23]De Bruyn W J,Clark C D,Ottelle K,et al.Photochemical degradation of phenanthrene as a function of natural water variables modeling freshwater to marine environments[J].Marine pollution bulletin,2012,64(3):532-538.
[24]杨凯,葛林科,那广水,等.水中噁唑烷酮类抗生素利奈唑酮的光化学行为[J].环境通报,2012,57(26):2469-2474.Yang K,Ge L K,Na G S,et al.Aqueous photochemical behavior of oxazolidinone antibiotic linezolid(in Chinese).Chin Sci Bull(Chin Ver),2012,57(26):2469-2474.
[25]Assel M,Laenen R,Laubereau A.Ultrafast electron trapping in an aqueous Na Cl-solution[J].Chemical Physics Letters,1998,289(3-4):267-274.
[26]Mostofa K M G,Sakugawa H.Spatial and temporal variations and factors controlling the concentrations of hydrogen peroxide and organic peroxides in rivers[J].Environmental Chemistry,2009,6(6):524-534.
[27]Brigante M,Minella M,Mailhot G,et al.Formation and reactivity of the dichloride radical(Cl2-)in surface waters:a modelling approach[J].Chemosphere,2014,95:464-469.
[28]Mack J,Bolton J.Photochemistry of nitrite and nitrate in aqueous solution:a review[J].Journal of Photochemistry and Photobiology A:Chemistry,1999,128(1-3):1-13.
[29]Zepp R,HoignéJ,Bader H.Nitrate-induced photooxidation of trace organic chemicals in water[J].Environmental Science and Technology,1987,21(5):443-450.
[30]Espinoza L,Neamtu M.The effect of nitrate,Fe(III)and bicarbonate on the degradation of bisphenol A by simulated solar-UV irradiation[J].Water Research,2007,41(19):4479-4487.
[31]Lin A Y C,Wang X H,Lee W N.Phototransformation determines the fate of 5-fluorouracil and cyclophosphamide in natural surface waters[J].Environmental Science and Technology,2013,47(9):4104-4112.
[32]Vione D,Falletti G,Maurino V,et al.Sources and Sinks of Hydroxyl Radicals upon Irradiation of Natural Water Samples[J].Environmental Science and Technology,2006,40(12):3775-3781.
[33]Wu C,Linden K G.Phototransformation of selected organophosphorus pesticides:roles of hydroxyl and carbonate radicals[J].Water Research,2010,44(12):3585-3594.