水体中磺胺甲噁唑间接光降解作用
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摘要
间接光降解是水体药物类污染物的主要去除途径之一,而有色溶解有机物(CDOM)是间接光降解的主要参与者.CDOM经过光照作用后产生大量活性中间体,与药物类污染物进行反应,完成间接光降解.本文着重研究了4种来源不同的CDOM对磺胺甲噁唑(SMZ)的间接光解作用和影响因素.结果表明,CDOM对于SMZ具有显著间接光降解作用,这种间接光降解具有双重性,既可以通过生成各种活性中间体来促进SMZ的间接光降解,又可以通过光屏蔽作用以及活性中间体掩蔽作用抑制SMZ的光降解.SMZ的间接光降解主要由CDOM产生的3CDOM*、HO·、1O2等活性中间体控制,其中3CDOM*为SMZ间接光降解的主要参与者.另外,pH、盐度和硝酸根离子对SMZ的间接光降解均具有显著影响作用,而碳酸氢根离子对于SMZ间接光降解的影响作用不明显.
Indirect photodegradation is one of the primary approaches for the removal of pharmaceutical contaminants from water.This degradation process is dominated by chromophoric dissolved organic matter(CDOM).After illumination,CDOM produces many reactive intermediates,which can react with drug pollutants to achieve indirect photodegradation.In this article,we focused on four different sources of CDOM and factors affecting indirect sulfamethoxazole(SMZ) photolysis.The results show that the indirect photodegradation effect of SMZ is significantly influenced by CDOM.This indirect photodegradation has a dual nature.It promotes the indirect photodegradation of SMZ through the formation of various reactive intermediates and at the same time inhibits the photodegradation of SMZ through light shielding and masking of reactive intermediates.The indirect photodegradation of SMZ is mainly controlled by active intermediates such as3 CDOM*,HO·,and 1O2 produced by CDOM;3 CDOM*is the main participant in indirect photodegradation of SMZ.In addition,the pH,salinity,and nitrate ions have a significant effect on the indirect photodegradation of SMZ,while bicarbonate ions have no significant effect on the indirect photodegradation of SMZ.
Indirect photodegradation is one of the primary approaches for the removal of pharmaceutical contaminants from water.This degradation process is dominated by chromophoric dissolved organic matter(CDOM).After illumination,CDOM produces many reactive intermediates,which can react with drug pollutants to achieve indirect photodegradation.In this article,we focused on four different sources of CDOM and factors affecting indirect sulfamethoxazole(SMZ) photolysis.The results show that the indirect photodegradation effect of SMZ is significantly influenced by CDOM.This indirect photodegradation has a dual nature.It promotes the indirect photodegradation of SMZ through the formation of various reactive intermediates and at the same time inhibits the photodegradation of SMZ through light shielding and masking of reactive intermediates.The indirect photodegradation of SMZ is mainly controlled by active intermediates such as3 CDOM*,HO·,and 1O2 produced by CDOM;3 CDOM*is the main participant in indirect photodegradation of SMZ.In addition,the pH,salinity,and nitrate ions have a significant effect on the indirect photodegradation of SMZ,while bicarbonate ions have no significant effect on the indirect photodegradation of SMZ.
引文
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[16]Chen Y,Hu C,Hu X X,et al.Indirect photodegradation of amine drugs in aqueous solution under simulated sunlight[J].Environmental Science&Technology,2009,43(8):2760-2765.
[17]Dubbini A,Censi R,Martena V,et al.Influence of p H and method of crystallization on the solid physical form of indomethacin[J].International Journal of Pharmaceutics,2014,473(1-2):536-544.
[18]Mc Cabe A J,Arnold W A.Reactivity of triplet excited states of dissolved natural organic matter in stormflow from mixed-use watersheds[J].Environmental Science&Technology,2017,51(17):9718-9728.
[19]Chen Y,Jiang X,Xiao K K,et al.Enhanced volatile fatty acids(VFAs)production in a thermophilic fermenter with stepwise pHincrease-investigation on dissolved organic matter transformation and microbial community shift[J].Water Research,2017,112:261-268.
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[25]Osburn C L,O'Sullivan D W,Boyd T J.Increases in the longwave photobleaching of chromophoric dissolved organic matter in coastal waters[J].Limnology and Oceanography,2009,54(1):145-159.
[26]Anastasio C,Newberg J T.Sources and sinks of hydroxyl radical in sea-salt particles[J].Journal of Geophysical Research,2007,112(D10):D10306.
[27]Mack J,Bolton J R.Photochemistry of nitrite and nitrate in aqueous solution:a review[J].Journal of Photochemistry and Photobiology A:Chemistry,1999,128(1-3):1-13.
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[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&Technology,2013,47(9):4104-4112.
[2]Vione D,Minella M,Maurino V,et al.Indirect photochemistry in sunlit surface waters:photoinduced production of reactive transient species[J].Chemistry:A European Journal,2014,20(34):10590-10606.
[3]Remucal C K,Ginder-Vogel M.A critical review of the reactivity of manganese oxides with organic contaminants[J].Environmental Science:Processes&Impacts,2014,16(6):1247-1266.
[4]Sharpless C M,Blough N V.The importance of charge-transfer interactions in determining chromophoric dissolved organic matter(CDOM)optical and photochemical properties[J].Environmental Science:Processes&Impacts,2014,16(4):654-671.
[5]TrovóA G,Nogueira R F P,Agüera A,et al.Photodegradation of sulfamethoxazole in various aqueous media:persistence,toxicity and photoproducts assessment[J].Chemosphere,2009,77(10):1292-1298.
[6]Xu H M,Cooper W J,Jung J,et al.Photosensitized degradation of amoxicillin in natural organic matter isolate solutions[J].Water Research,2011,45(2):632-638.
[7]Yang W L,Ben Abdelmelek S,Zheng Z,et al.Photochemical transformation of terbutaline(pharmaceutical)in simulated natural waters:degradation kinetics and mechanisms[J].Water Research,2013,47(17):6558-6565.
[8]Porras J,Bedoya C,Silva-Agredo J,et al.Role of humic substances in the degradation pathways and residual antibacterial activity during the photodecomposition of the antibiotic ciprofloxacin in water[J].Water Research,2016,94:1-9.
[9]Zhang S Y,Chen J W,Xie Q,et al.Comment on“Effect of dissolved organic matter on the transformation of contaminants induced by excited triplet states and the hydroxyl radical”[J].Environmental Science&Technology,2011,45(18):7945-7946.
[10]Bahnmüller S,Von Gunten U,Canonica S.Sunlight-induced transformation of sulfadiazine and sulfamethoxazole in surface waters and wastewater effluents[J].Water Research,2104,57:183-192.
[11]Ryan C C,Tan D T,Arnold W A.Direct and indirect photolysis of sulfamethoxazole and trimethoprim in wastewater treatment plant effluent[J].Water Research,2011,45(3):1280-1286.
[12]Mc Kay G,Couch K D,Mezyk S P,et al.Investigation of the coupled effects of molecular weight and charge-transfer interactions on the optical and photochemical properties of dissolved organic matter[J].Environmental Science&Technology,2016,50(15):8093-8102.
[13]Li R,Zhao C,Yao B,et al.Photochemical transformation of aminoglycoside antibiotics in simulated natural waters[J].Environmental Science&Technology,2016,50(6):2921-2930.
[14]Wenk J,Canonica S.Phenolic antioxidants inhibit the tripletinduced transformation of anilines and sulfonamide antibiotics in aqueous solution[J].Environmental Science&Technology,2012,46(10):5455-5462.
[15]Kieber R J,Zhou X L,Mopper K.Formation of carbonyl compounds from UV-induced photodegradation of humic substances in natural waters:fate of riverine carbon in the sea[J].Limnology and Oceanography,1990,35(7):1503-1515.
[16]Chen Y,Hu C,Hu X X,et al.Indirect photodegradation of amine drugs in aqueous solution under simulated sunlight[J].Environmental Science&Technology,2009,43(8):2760-2765.
[17]Dubbini A,Censi R,Martena V,et al.Influence of p H and method of crystallization on the solid physical form of indomethacin[J].International Journal of Pharmaceutics,2014,473(1-2):536-544.
[18]Mc Cabe A J,Arnold W A.Reactivity of triplet excited states of dissolved natural organic matter in stormflow from mixed-use watersheds[J].Environmental Science&Technology,2017,51(17):9718-9728.
[19]Chen Y,Jiang X,Xiao K K,et al.Enhanced volatile fatty acids(VFAs)production in a thermophilic fermenter with stepwise pHincrease-investigation on dissolved organic matter transformation and microbial community shift[J].Water Research,2017,112:261-268.
[20]Garoma T,Umamaheshwar S K,Mumper A.Removal of sulfadiazine,sulfamethizole,sulfamethoxazole,and sulfathiazole from aqueous solution by ozonation[J].Chemosphere,2010,79(8):814-820.
[21]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.
[22]Yang Y,Pignatello J J,Ma J,et al.Comparison of halide impacts on the efficiency of contaminant degradation by sulfate and hydroxyl radical-based advanced oxidation processes(AOPs)[J].Environmental Science&Technology,2014,48(4):2344-2351.
[23]Formosinho S J,Arnaut L G.Some new perspectives on electron transfer reactions through the intersecting-state model[J].Journal of Photochemistry and Photobiology A:Chemistry,1994,82(1-3):11-29.
[24]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.
[25]Osburn C L,O'Sullivan D W,Boyd T J.Increases in the longwave photobleaching of chromophoric dissolved organic matter in coastal waters[J].Limnology and Oceanography,2009,54(1):145-159.
[26]Anastasio C,Newberg J T.Sources and sinks of hydroxyl radical in sea-salt particles[J].Journal of Geophysical Research,2007,112(D10):D10306.
[27]Mack J,Bolton J R.Photochemistry of nitrite and nitrate in aqueous solution:a review[J].Journal of Photochemistry and Photobiology A:Chemistry,1999,128(1-3):1-13.
[28]Wagner I,Strehlow H,Busse G.Flash photolysis of nitrate ions in aqueous solution[J].Zeitschrift für Physikalische Chemie,1980,123(1):1-33.
[29]Zafiriou O C,True M B.Nitrite photolysis in seawater by sunlight[J].Marine Chemistry,1979,8(1):9-32.
[30]Ross F,Ross,A B.Selected specific rates of reactions of transients from water in aqueous solution;ⅢHydroxylradical and perhydroxyl radical ions[M].NSRDS-NBS 59.National Bureau of Standards,Washington,D.C.,US Government Printing Office,1977.
[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&Technology,2013,47(9):4104-4112.