UV和UV/H_2O_2工艺对水中二嗪磷的降解
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摘要
在低压汞灯(LPUV,253.7nm)光照条件下,研究了过氧化氢(H_2O_2)加入量对二嗪磷降解动力学、产物生成和降解途径的影响规律与作用机理.结果表明,二嗪磷水溶液在单独UV和UV/H_2O_2工艺中的降解反应均符合准一级反应动力学,且反应速率常数(k)随H_2O_2加入量的增加而增大,H_2O_2加入量为0,5,10mg/L时的k分别为0.0234,0.0301,0.0341min~(–1).在UV光照处理条件下,二嗪磷水溶液中的溶解性有机碳(DOC)随H_2O_2加入量的增加而降低,但其矿化度均相对较低(光照120min时的DOC去除率均低于20%).此外,UV光照处理时,H_2O_2的加入对二嗪磷光氧化降解产物的种类及生成量均存在显著影响.二嗪磷水溶液单独UV光照处理60min时检出了8种中间/降解产物,但经UV/H_2O_2工艺处理60min时仅检出了6种中间/降解产物,且不同H_2O_2加入量时的光氧化降解产物生成量或浓度及随UV光照处理时间的变化幅度与趋势均存在较大程度的差别.基于二嗪磷及其降解产物的定性、(半)定量分析结果,提出了二嗪磷水溶液在单独UV和UV/H_2O_2工艺中的降解途径与机理.
The degradation kinetics, intermediates formation and degradation pathway of diazinon at different dosages of H_2O_2 under ultraviolet(UV) irradiation(253.7 nm) was investigated. The results showed that H_2O_2 significantly affected on the photo-degradation rate of diazinon in UV irradiation treatment processes. The rate was lower under sole UV treatment(the pseudo-first-order rate constant(k) was 0.0234 min~(-1)) than UV/H_2O_2 treatment with H_2O_2 dose of 5 and 10 mg/L(k=0.0301 min~(-1) and k=0.0341 min~(-1),respectively). More than 94% of diazinon was degraded within 120 min of UV irradiation during sole UV and UV/H_2O_2 treatment processes. In addition, dissolved organic carbon(DOC) in diazinon aqueous solution decreased with the dosage of H_2O_2 increased from 0 to 10 mg/L under the UV irradiation treatment. However, the removal efficiency of DOC was relatively low, which was less than 20% within 120 min of UV irradiation during all treatment conditions in this study. The degradation intermediates of diazinon varied significantly under different H_2O_2 dosages. Eight major species of degradation intermediates were detected after 60 minutes of sole UV irradiation, while only six species were detected after 60 minutes of the UV/H_2O_2 oxidation treatment. A systematic qualitative and semiquantitative analyses of the intermediates of diazinon under different H_2O_2 dosages were conducted, the degradation pathways of diazinon during the sole UV and UV/H_2O_2 treatment processes were discussed as well.
The degradation kinetics, intermediates formation and degradation pathway of diazinon at different dosages of H_2O_2 under ultraviolet(UV) irradiation(253.7 nm) was investigated. The results showed that H_2O_2 significantly affected on the photo-degradation rate of diazinon in UV irradiation treatment processes. The rate was lower under sole UV treatment(the pseudo-first-order rate constant(k) was 0.0234 min~(-1)) than UV/H_2O_2 treatment with H_2O_2 dose of 5 and 10 mg/L(k=0.0301 min~(-1) and k=0.0341 min~(-1),respectively). More than 94% of diazinon was degraded within 120 min of UV irradiation during sole UV and UV/H_2O_2 treatment processes. In addition, dissolved organic carbon(DOC) in diazinon aqueous solution decreased with the dosage of H_2O_2 increased from 0 to 10 mg/L under the UV irradiation treatment. However, the removal efficiency of DOC was relatively low, which was less than 20% within 120 min of UV irradiation during all treatment conditions in this study. The degradation intermediates of diazinon varied significantly under different H_2O_2 dosages. Eight major species of degradation intermediates were detected after 60 minutes of sole UV irradiation, while only six species were detected after 60 minutes of the UV/H_2O_2 oxidation treatment. A systematic qualitative and semiquantitative analyses of the intermediates of diazinon under different H_2O_2 dosages were conducted, the degradation pathways of diazinon during the sole UV and UV/H_2O_2 treatment processes were discussed as well.
引文
[1]刘玉灿,苏苗苗,张岩,等.溶液制备过程引入的甲醇对阿特拉津UV光氧化速率和降解机理的影响[J].化学学报,2019,7(1):72-83.Liu Y C,Su M M,Zhang Y,et al.Influence rule of organic solvents methanol from sample preparation on degradation rate and mechanism of atrazine in UV-based oxidation processes[J].Acta Chimica Sinica,2019,77(1):72-83.
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[13]Fadaei A M,Dehghani M H,Mahvi A H,et al.Degradation of organophosphorus pesticides in water during UV/H2O2 treatment:role of sulphate and bicarbonate ions[J].Journal of Chemistry,2012,9(4):2015-2022.
[14]Ikehata K,El-Din M G.Aqueous pesticide degradation by hydrogen peroxide/ultraviolet irradiation and Fenton-type advanced oxidation processes:a review[J].Journal of Environmental Engineering and Science,2006,5(2):81-135.
[15]Clark K K,Mezyk S P,Abbott A,et al.Kinetic studies of the AOPradical-based oxidative and reductive destruction of pesticides and model compounds in water[J].Chemosphere,2018,197:193-199.
[16]Kouloumbos V N,Tsipi D F,Hiskia A E,et al.Identification of photocatalytic degradation products of diazinon in Ti O2aqueous suspensions using GC/MS/MS and LC/MS with quadrupole time-offlight mass spectrometry[J].Journal of the American Society for Mass Spectrometry,2003,14(8):803-817.
[17]Sancho J V,PozoóJ,Ibá?ez M,et al.Potential of liquid chromatography/time-of-flight mass spectrometry for the determination of pesticides and transformation products in water[J].Analytical and Bioanalytical Chemistry,2006,386(4):987-997.
[18]?olovi?M,Krsti?D,Petrovi?S,et al.Toxic effects of diazinon and its photodegradation products[J].Toxicology Letters,2010,193(1):9-18.
[19]Ku Y,Chang J L,Cheng S C.Effect of solution pH on the hydrolysis and photolysis of diazinon in aqueous solution[J].Water,Air,and Soil Pollution,1998,108(3/4):445-456.
[20]Jonidi-Jafari A,Gholami M,Farzadkia M,et al.Application of Ni-doped ZnO nanorods for degradation of diazinon:Kinetics and by-products[J].Separation Science and Technology,2017,52(15):2395-2406.
[21]Souza A G,Cardeal Z L,Augusti R.Electrospray Ionization Mass Spectrometry(ESI-MS)monitoring of the photolysis of diazinon in aqueous solution:Degradation route and toxicity of by-products against Artemia salina[J].Journal of Environmental Science and Health,Part B,2013,48(3):171-176.
[22]Nakaoka Y,Katsumata H,Kaneco S,et al.Photocatalytic degradation of diazinon in aqueous solution by platinized TiO2[J].Desalination and Water Treatment,2010,13(1-3):427-436.
[2]Wang D,Singhasemanon N,Goh K S.A review of diazinon use,contamination in surface waters,and regulatory actions in California across water years 1992-2014[J].Environmental Monitoring and assessment,2017,189(7):310-316.
[3]Ogasawara N,Matsushima M,Kawamura N,et al.Modulation of immunological activity on macrophages induced by diazinon[J].Toxicology,2017,379:22-30.
[4]Velki M,Meyer Alert H,Seiler T B,et al.Enzymatic activity and gene expression changes in zebrafish embryos and larvae exposed to pesticides diazinon and diuron[J].Aquatic Toxicology,2017,193:187-200.
[5]Parker A M,Lester Y,Spangler E K,et al.UV/H2O2 advanced oxidation for abatement of organophosphorous pesticides and the effects on various toxicity screening assays[J].Chemosphere,2017,182:477-482.
[6]Real F J,Benitez F J,Acero J L,et al.Removal of diazinon by various advanced oxidation processes[J].Journal of Chemical Technology&Biotechnology:International Research in Process,Environmental&Clean Technology,2007,82(6):566-574.
[7]Reddy P V L,Kim K H.A review of photochemical approaches for the treatment of a wide range of pesticides[J].Journal of Hazardous materials,2015,285:325-335.
[8]Oturan M A,Aaron J J.Advanced oxidation processes in water/wastewater treatment:principles and applications.A review[J].Critical Reviews in Environmental Science and Technology,2014,44(23):2577-2641.
[9]Reddy P V L,Kim K H.A review of photochemical approaches for the treatment of a wide range of pesticides[J].Journal of Hazardous Materials,2015,285:325-335.
[10]Shemer H,Linden K G.Degradation and by-product formation of diazinon in water during UV and UV/H2O2 treatment[J].Journal of Hazardous Materials,2006,136(3):553-559.
[11]Lekkerkerker Teunissen K,Benotti M J,Snyder S A,et al.Transformation of atrazine,carbamazepine,diclofenac and sulfamethoxazole by low and medium pressure UV and UV/H2O2treatment[J].Separation and Purification Technology,2012,96:33-43.
[12]刘玉灿,段晋明,李伟.溶液pH值对二嗪磷紫外光降解产物及降解途径的影响[J].化学学报,2015,73(11):1196-1202.Liu Y C,Duan J M,Li W.Influence of solution pH on photolysis intermediates and degradation pathway of diazinon during UVirradiation treatment[J].Acta Chimica Sinica,2015,73(11):1196-1202.
[13]Fadaei A M,Dehghani M H,Mahvi A H,et al.Degradation of organophosphorus pesticides in water during UV/H2O2 treatment:role of sulphate and bicarbonate ions[J].Journal of Chemistry,2012,9(4):2015-2022.
[14]Ikehata K,El-Din M G.Aqueous pesticide degradation by hydrogen peroxide/ultraviolet irradiation and Fenton-type advanced oxidation processes:a review[J].Journal of Environmental Engineering and Science,2006,5(2):81-135.
[15]Clark K K,Mezyk S P,Abbott A,et al.Kinetic studies of the AOPradical-based oxidative and reductive destruction of pesticides and model compounds in water[J].Chemosphere,2018,197:193-199.
[16]Kouloumbos V N,Tsipi D F,Hiskia A E,et al.Identification of photocatalytic degradation products of diazinon in Ti O2aqueous suspensions using GC/MS/MS and LC/MS with quadrupole time-offlight mass spectrometry[J].Journal of the American Society for Mass Spectrometry,2003,14(8):803-817.
[17]Sancho J V,PozoóJ,Ibá?ez M,et al.Potential of liquid chromatography/time-of-flight mass spectrometry for the determination of pesticides and transformation products in water[J].Analytical and Bioanalytical Chemistry,2006,386(4):987-997.
[18]?olovi?M,Krsti?D,Petrovi?S,et al.Toxic effects of diazinon and its photodegradation products[J].Toxicology Letters,2010,193(1):9-18.
[19]Ku Y,Chang J L,Cheng S C.Effect of solution pH on the hydrolysis and photolysis of diazinon in aqueous solution[J].Water,Air,and Soil Pollution,1998,108(3/4):445-456.
[20]Jonidi-Jafari A,Gholami M,Farzadkia M,et al.Application of Ni-doped ZnO nanorods for degradation of diazinon:Kinetics and by-products[J].Separation Science and Technology,2017,52(15):2395-2406.
[21]Souza A G,Cardeal Z L,Augusti R.Electrospray Ionization Mass Spectrometry(ESI-MS)monitoring of the photolysis of diazinon in aqueous solution:Degradation route and toxicity of by-products against Artemia salina[J].Journal of Environmental Science and Health,Part B,2013,48(3):171-176.
[22]Nakaoka Y,Katsumata H,Kaneco S,et al.Photocatalytic degradation of diazinon in aqueous solution by platinized TiO2[J].Desalination and Water Treatment,2010,13(1-3):427-436.
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