丰枯水期鄱阳湖表层水中羟基自由基浓度及其抗生素净化作用研究
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摘要
鄱阳湖位于我国农业大省江西省,表层湖水中羟基自由基(HO·)引发的水体光化学反应,可能对流域内的农业污染物—抗生素具有潜在的净化作用.因此,本研究以氙灯模拟太阳光测得鄱阳湖及周边河流羟基自由基表观光量子产率(ΦHO·),在丰水期为(0.57~10.33)×10~(-5),枯水期为(0.45~3.52)×10~(-5).丰水期溶解态有机物(DOM)对HO·形成的贡献率为85.8%~98.7%,枯水期为58.5%~97.6%,表明DOM是HO·形成的主导物质.可能由于水体混合均匀,丰水期除抚河水体可能有其特殊的化学组成外,其它湖泊与河流的水化学组成接近,表现出随溶解态有机碳含量升高,ΦHO·呈先增大后减小的现象.枯水期水体各化学组成含量显著高于丰水期,光屏蔽与淬灭可能起主要作用,只有当NO_2~-含量较高时才显示出对HO·形成的贡献.依据太阳光强可得鄱阳湖丰水期及枯水期表层水HO·的稳态浓度分别为9.51×10~(-16)与4.92×10~(-17)mol·L~(-1),湖水中5种抗生素在HO·作用下的半衰期分别为2.3~13.9 d与44.5~268.7 d,丰水期鄱阳湖表现出更高的光化学净化能力.
Poyang Lake,which located in Jiangxi Province,could play an important role in purifying domestic antibiotic pollutants by hydroxyl radicals( HO·) formed in surface waters through photochemical reactions.The present study showed that the apparent quantum yields of hydroxyl radical( ΦHO·)in Poyang Lake as well as its surrounding rivers were estimated to be( 0.57 ~ 10.33) ×10~(-5) in wet season and( 0.45 ~ 3.52) ×10~(-5) in dry season,and the dissolved organic matter( DOM) contribute 85.8% ~ 98.7% and 58.5% ~ 97.6% to the formation of HO·in wet and dry seasons respectively,suggesting that DOM was the main source of HO·. In wet season,the chemical properties in sampling sites were similar except for Fu River,probably due to the strengthened hydrodynamic connectivity between different water bodies.With the increase of dissolved organic carbon,ΦHO· was firstly increased and then decreased.In dry season,significantly higher levels of dissolved chemicals were obtained,which primarily presented strong light screening and radical quenching effects towards HO·.While the contribution of NO_2~- to HO·could only been observed at high NO_2~- levels.The averaged steady concentrations of HO·in Poyang Lake was estimated to be 9.51×10~(-16) and 4.92×10~(-17) mol·L~(-1) in wet and dry seasons according to ΦHO· and intensity of solar irradiation,respectively.Hence,the half-lives of five antibiotics in Poyang Lake were evaluated to be 2.3 ~ 13.9 and 44.5 ~ 268.7 days attributed to the degradation by HO·,indicating the higher efficient purification of antibiotics pollutants in Poyang Lake during wet season.
Poyang Lake,which located in Jiangxi Province,could play an important role in purifying domestic antibiotic pollutants by hydroxyl radicals( HO·) formed in surface waters through photochemical reactions.The present study showed that the apparent quantum yields of hydroxyl radical( ΦHO·)in Poyang Lake as well as its surrounding rivers were estimated to be( 0.57 ~ 10.33) ×10~(-5) in wet season and( 0.45 ~ 3.52) ×10~(-5) in dry season,and the dissolved organic matter( DOM) contribute 85.8% ~ 98.7% and 58.5% ~ 97.6% to the formation of HO·in wet and dry seasons respectively,suggesting that DOM was the main source of HO·. In wet season,the chemical properties in sampling sites were similar except for Fu River,probably due to the strengthened hydrodynamic connectivity between different water bodies.With the increase of dissolved organic carbon,ΦHO· was firstly increased and then decreased.In dry season,significantly higher levels of dissolved chemicals were obtained,which primarily presented strong light screening and radical quenching effects towards HO·.While the contribution of NO_2~- to HO·could only been observed at high NO_2~- levels.The averaged steady concentrations of HO·in Poyang Lake was estimated to be 9.51×10~(-16) and 4.92×10~(-17) mol·L~(-1) in wet and dry seasons according to ΦHO· and intensity of solar irradiation,respectively.Hence,the half-lives of five antibiotics in Poyang Lake were evaluated to be 2.3 ~ 13.9 and 44.5 ~ 268.7 days attributed to the degradation by HO·,indicating the higher efficient purification of antibiotics pollutants in Poyang Lake during wet season.
引文
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刘雪石,乔显亮,刘远.2017.DOM的光化学活性及其对污染物光解的影响[J].环境科学与技术,40(1):85-94
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Vione D,Minero C,Maurino V,et al.2007.Seasonal and water column trends of the relative role of nitrate and nitrite as HO·sources in surface waters[J].Annali Di Chimica,97(8):699-711
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许磊,李华,陈英旭,等.2010.南太湖地区小型浅水湖泊自净能力季节变化研究[J].环境科学,31(4):924-930
杨岳主,李玉平,杨道武,等.2013.铁铜催化剂非均相Fenton降解苯酚及机制研究[J].环境科学,34(7):2658-2664
Zeng T,Arnold W A.2013.Pesticide photolysis in Prairie Potholes:Probing photosensitized processes[J].Environmental Science&Technology,47(13):6735-6745
Zhang D N,Yan S W,Song W H.2014.Photochemically induced formation of reactive oxygen species(ROS)from effluent organic matter[J].Environmental Science&Technology,48(21):12645-12653
Zhang Q Q,Ying G G,Pan C G,et al.2015.Comprehensive evaluation of antibiotics emission and fate in the river basins of China:Source analysis,multimedia modeling,and linkage to bacterial resistance[J].Environmental Science&Technology,49(11):6772-6782
赵群.2014.药物及个人护理品在水中光解的研究进展[J].山东理工大学学报(自然科学版),28(3):73-78
郑晓冬,乔显亮,肖杰,等.2013.水中溶解性有机质对三氯生光解的影响[J].环境科学与技术,36(10):182-185
Chen B W,Liang X M,Huang X P,et al.2013.Differentiating anthropogenic impacts on ARGs in the Pearl River estuary by using suitable gene indicators[J].Water Research,47(8):2811-2820
Cheng D M,Liu X H,Zhao S N,et al.2017.Influence of the natural colloids on the multi-phase distributions of antibiotics in the surface water from the largest lake in North China[J].Science of the Total Environment,578:649-659
Ding H J,Wu Y X,Zhang W H,et al.2017.Occurrence,distribution,and risk assessment of antibiotics in the surface water of Poyang Lake,the largest freshwater lake in China[J].Chemosphere,184:137-147
Dulin D,Mill T.1982.Development and evaluation of sunlight actinometers[J].Environmental Science&Technology,16(11):815-820
Egli T.2010.How to live at very low substrate concentration[J].Water Research,44(17):4826-4837
Fan Q Z,Zhang Y,Ma W C,et al.2016.Spatial and seasonal dynamics of ship emissions over the Yangtze River Delta and East China Sea and their potential environmental influence[J].Environmental Science&Technology,50(3):1322-1329
Fang H S,Gao Y P,Wang H H,et al.2017.Photo-induced oxidative damage to dissolved free amino acids by the photosensitizer polycyclic musk tonalide:Transformation kinetics and mechanisms[J].Water Research,115(Supplement C):339-346
Fenner K,Canonica S,Wackett L P,et al.2013.Evaluating pesticide degradation in the environment:Blind spots and emerging opportunities[J].Science,341(6147):752-758
Ge L K,Na G S,Zhang S Y,et al.2015.New insights into the aquatic photochemistry of fluoroquinolone antibiotics:Direct photodegradation,hydroxyl-radical oxidation,and antibacterial activity changes[J].Science of the Total Environment,527-528(Supplement C):12-17
胡振鹏,张祖芳,刘以珍,等.2015.碟形湖在鄱阳湖湿地生态系统的作用和意义[J].江西水利科技,41(5):317-323
黄建,田森林,李英杰.2017.药物和个人护理品的水环境光化学转化动力学研究[J].环境科学导刊,36(增刊):37-40
Jankowski J J,Kieber D J,Mopper K.1999.Nitrate and nitrite ultraviolet actinometers[J].Photochemistry and Photobiology,70(3):319-328
Lapertot M,Pulgarín C,Fernández-Ibá1ez P,et al.2006.Enhancing biodegradability of priority substances(pesticides)by solar photoFenton[J].Water Research,40(5):1086-1094
Li K,Zhang P,Ge L K,et al.2014.Concentration-dependent photodegradation kinetics and hydroxyl-radical oxidation of phenicol antibiotics[J].Chemosphere,111(Supplement C):278-282
Liang X M,Chen B W,Nie X P,et al.2013.The distribution and partitioning of common antibiotics in water and sediment of the Pearl River estuary,south China[J].Chemosphere,92(11):1410-1416
刘雪石,乔显亮,刘远.2017.DOM的光化学活性及其对污染物光解的影响[J].环境科学与技术,40(1):85-94
Ma R X,Wang B,Lu S Y,et al.2016.Characterization of pharmaceutically active compounds in Dongting Lake,China:Occurrence,chiral profiling and environmental risk[J].Science of the Total Environment,557-558:268-275
Page S E,Kling G W,Sander M,et al.2013.Dark formation of hydroxyl radical in arctic soil and surface waters[J].Environmental Science&Technology,47(22):12860-12867
唐昌新,熊雄,邬年华,等.2015.长江倒灌对鄱阳湖水动力特征影响的数值模拟[J].湖泊科学,27(4):700-710
Vione D,Minero C,Maurino V,et al.2007.Seasonal and water column trends of the relative role of nitrate and nitrite as HO·sources in surface waters[J].Annali Di Chimica,97(8):699-711
Wols B A,Harmsen D J H,Beerendonk E F,et al.2014.Predicting pharmaceutical degradation by UV(LP)/H2O2processes:A kinetic model[J].Chemical Engineering Journal,255(Supplement C):334-343
许磊,李华,陈英旭,等.2010.南太湖地区小型浅水湖泊自净能力季节变化研究[J].环境科学,31(4):924-930
杨岳主,李玉平,杨道武,等.2013.铁铜催化剂非均相Fenton降解苯酚及机制研究[J].环境科学,34(7):2658-2664
Zeng T,Arnold W A.2013.Pesticide photolysis in Prairie Potholes:Probing photosensitized processes[J].Environmental Science&Technology,47(13):6735-6745
Zhang D N,Yan S W,Song W H.2014.Photochemically induced formation of reactive oxygen species(ROS)from effluent organic matter[J].Environmental Science&Technology,48(21):12645-12653
Zhang Q Q,Ying G G,Pan C G,et al.2015.Comprehensive evaluation of antibiotics emission and fate in the river basins of China:Source analysis,multimedia modeling,and linkage to bacterial resistance[J].Environmental Science&Technology,49(11):6772-6782
赵群.2014.药物及个人护理品在水中光解的研究进展[J].山东理工大学学报(自然科学版),28(3):73-78
郑晓冬,乔显亮,肖杰,等.2013.水中溶解性有机质对三氯生光解的影响[J].环境科学与技术,36(10):182-185