MnO_2对酰胺类除草剂乙基磺酸转化产物(ESA)的去除
|
摘要
酰胺类除草剂是目前使用最多、最广泛的一类芽前除草剂,而其乙基磺酸转化产物(ESA)具有更大的环境持久性,因此ESA的去除具有显著的环境意义。研究了化学合成的MnO_2对ESA的吸附-氧化行为,并且考察了MnO_2初始浓度、体系初始pH值以及共存金属离子等因素对ESA去除效率的影响。结果表明:ESA能被MnO_2有效地去除,同时ESA的去除效率随着MnO_2初始浓度的增大而增大;且酸性条件更有利于MnO_2对ESA的去除,而溶液中的共存金属离子会对去除产生抑制作用,且Fe3+抑制效应最大。
Amide herbicides are one of the most applied herbicides at present,and their ethylsulfonic acid-converted products(ESA)have long-lasting influences on environment.Therefore,adsorption-oxidative degradation of the ESA by MnO_2 was investigated in this study.Influences of initial concentration of the MnO_2,initial pH value and simultaneously presented metal ions on the removal efficiency of ESA were discussed.The results showed that the ESA was degraded by MnO_2 efficiently in aqueous solutions,and the increase of initial concentration of MnO_2 led to an increased ESA remove efficiency.In addition,the efficiency of of ESA removal increased as decreasing pH values,suggesting that the acidic conditions was favorable to the removal of ESA.The simultaneously presented metal ions had inhibitory effect on the removal of ESA with Fe3+ had greater effect than Na+ and Ca2+.
Amide herbicides are one of the most applied herbicides at present,and their ethylsulfonic acid-converted products(ESA)have long-lasting influences on environment.Therefore,adsorption-oxidative degradation of the ESA by MnO_2 was investigated in this study.Influences of initial concentration of the MnO_2,initial pH value and simultaneously presented metal ions on the removal efficiency of ESA were discussed.The results showed that the ESA was degraded by MnO_2 efficiently in aqueous solutions,and the increase of initial concentration of MnO_2 led to an increased ESA remove efficiency.In addition,the efficiency of of ESA removal increased as decreasing pH values,suggesting that the acidic conditions was favorable to the removal of ESA.The simultaneously presented metal ions had inhibitory effect on the removal of ESA with Fe3+ had greater effect than Na+ and Ca2+.
引文
[1]TSAFTARIS A.The development of herbicide-tolerant transgenic crops[J].Field crops research,1996,45(1):115-123.
[2]张安平,吕立,孙建强,等.温室中有机氯农药残留及其对映体选择性研究[J].浙江工业大学学报,2016,44(6):639-644.
[3]周炳,赵美蓉,黄海凤.4种农药对斑马鱼胚胎的毒理研究[J].浙江工业大学学报,2008,36(2):136-140.
[4]黄伯俊.农药毒理一毒性手册[M].北京:人民卫生出版社,1993.
[5]杨彩霞,潘志彦,赵美蓉,等.类雌激素农药对雌性哺乳动物的生殖毒理研究[J].浙江工业大学学报,2008,36(2):122-128.
[6]ROBERTS T R,HUTSON D H,LEE P W,et al.Metabolic pathways of agrochemicals,part one:herbicides and plant growth regulators[M].Cambridge:The Royal Society of Chemistry,1998.
[7]ROBERTS T R,HUTSON D H,LEE P W.Metabolic pathways of agrochemicals,part two:insecticides and fungicides[M].Cambridge:The Royal Society of Chemistry,1999.
[8]AIZAWA H.Metabolic maps[M].San Diego:Academic Press,2001.
[9]COATS J R.What happens to degradable pesticides[J].Chemtech,1993,23(3):25-29.
[10]张建坤,赵晓亚,赵晖,等.酰胺类除草剂甲草胺的微生物降解研究进展[J].化学与生物工程,2009,26(6):19-23.
[11]FAVA L,BOTTONI P,CROBE A,et al.Leaching properties of some degradation products of alachlor and metolachlor[J].Chemosphere,2000,41(9):1503-1508.
[12]OSANO O,ADMIRAAL W,OTIENO D.Developmental disorders in embryos of the frog Xenopus laevis induced by chloroacetanilide herbicides and their degradation products[J].Environmental toxicology and chemistry,2002,21(2):375-379.
[13]SCRIBNER E A,THURMAN E M,ZIMMERMAN L R.Analysis of selected herbicide metabolites in surface and ground water of the United States[J].Science of the total environment,2000,248(2):157-167.
[14]赵玲.二氧化锰体系下氯酚的非生物转化研究[D].广州:中国科学院(广州地球化学研究所),2006.
[15]RUBERT K F,PEDERSEN J A.Kinetics of oxytetracycline reaction with a hydrous manganese oxide[J].Environmental science&technology,2006,40(23):7216-7221.
[16]SHINDO H,HUANG P M.Significance of Mn(IV)oxide in abiotic formation of organic nitrogen complexes in natural environments[J].Nature,1984,308(5954):57-58.
[17]JIANG L Y,HUANG C,CHEN J M,et al.Oxidative transformation of 17β-estradiol by MnO2in aqueous solution[J].Archives of environmental contamination&toxicology,2009,57(2):221-229.
[18]ZHANG H,HUANG C H.Oxidative transformation of triclosan and chlorophene by manganese oxides[J].Environmental science&technology,2003,37(11):2421-2430.
[19]JIN Y S,CHENEY M A.Abiotic transformation of atrazine in aqueous suspension of four synthetic manganese oxides[J].Colloids&surfaces a physicochemical&engineering aspects,2004,242(1/2/3):85-92.
[20]BALDWIN D S,AND J K B,COLEMAN L M,et al.Hydrolysis of an organophosphate ester by manganese dioxide[J].Environmental science&technology,2001,35(4):713-716.
[21]LAHA S,LUTHY R G.Oxidation of aniline and other primary aromatic amines by manganese dioxide[J].Environmental science&technology,1990,24,3(3):363-373.
[22]MURRAY J W.The surface chemistry of hydrous manganese dioxide[J].Journal of colloid and interface science,1974,46(3):357-371.
[23]CHEN G,ZHAO L,DONG Y H.Oxidative degradation kinetics and products of chlortetracycline by manganese dioxide[J].Journal of hazardous materials,2011,193(20):128-138.
[24]KLAUSEN J,AND S B H,SCHWARZENBACH R P.Oxidation of substituted anilines by aqueous MnO2:effect of cosolutes on initial and quasi-steady-state kinetics[J].Environmental science&technology,1997,31(9):2642-2649.
[25]GAO J,PEDERSEN J A.Adsorption of sulfonamide antimicrobial agents to clay minerals[J].Environmental science&technology,2005,39(24):9509-9516.
[26]PAROLO M E,SAVINI M C,VALLS J M,et al.Tetracycline adsorption on montmorillonite:pH and ionic strength effects[J].Applied clay science,2008,40(1/2/3/4):179-186.
[27]FORREZ I,CARBALLA M,VERBEKEN K,et al.Diclofenac oxidation by biogenic manganese oxides[J].Environmental science&technology,2010,44(9):3449-3454.
[28]CHEN W R,HUANG C H.Transformation kinetics and pathways of tetracycline antibiotics with manganese oxide[J].Environmental pollution,2011,159(5):1092-1100.
[29]刘涉江,李木金,姜斌,等.甲基叔丁基醚(MTBE)在不同粘性土壤中的吸附特性[J].环境工程学报,2007,1(1):110-112.
[30]KOSMULSKI M.The pH-dependent surface charging and the points of zero charge[J].Journal of colloid&interface science,2002,253(1):77-87.
[31]FORREZ I,CARBALLA M,NOPPE H,et al.Influence of manganese and ammonium oxidation on the removal of 17alpha-ethinylestradiol(EE2)[J].Water research,2009,43(1):77-86.
[32]BARRETT K A,MCBRIDE M B.Oxidative degradation of glyphosate and aminomethylphosphonate by manganese oxide[J].Environmental science&technology,2005,39(23):9223-9228.
[33]STONE A T,MORGAN J J.Reduction and dissolution of manganese(III)and manganese(IV)oxides by organics.1.reaction with hydroquinone[J].Environmental science&technology,1984,18(6):450-456.
[2]张安平,吕立,孙建强,等.温室中有机氯农药残留及其对映体选择性研究[J].浙江工业大学学报,2016,44(6):639-644.
[3]周炳,赵美蓉,黄海凤.4种农药对斑马鱼胚胎的毒理研究[J].浙江工业大学学报,2008,36(2):136-140.
[4]黄伯俊.农药毒理一毒性手册[M].北京:人民卫生出版社,1993.
[5]杨彩霞,潘志彦,赵美蓉,等.类雌激素农药对雌性哺乳动物的生殖毒理研究[J].浙江工业大学学报,2008,36(2):122-128.
[6]ROBERTS T R,HUTSON D H,LEE P W,et al.Metabolic pathways of agrochemicals,part one:herbicides and plant growth regulators[M].Cambridge:The Royal Society of Chemistry,1998.
[7]ROBERTS T R,HUTSON D H,LEE P W.Metabolic pathways of agrochemicals,part two:insecticides and fungicides[M].Cambridge:The Royal Society of Chemistry,1999.
[8]AIZAWA H.Metabolic maps[M].San Diego:Academic Press,2001.
[9]COATS J R.What happens to degradable pesticides[J].Chemtech,1993,23(3):25-29.
[10]张建坤,赵晓亚,赵晖,等.酰胺类除草剂甲草胺的微生物降解研究进展[J].化学与生物工程,2009,26(6):19-23.
[11]FAVA L,BOTTONI P,CROBE A,et al.Leaching properties of some degradation products of alachlor and metolachlor[J].Chemosphere,2000,41(9):1503-1508.
[12]OSANO O,ADMIRAAL W,OTIENO D.Developmental disorders in embryos of the frog Xenopus laevis induced by chloroacetanilide herbicides and their degradation products[J].Environmental toxicology and chemistry,2002,21(2):375-379.
[13]SCRIBNER E A,THURMAN E M,ZIMMERMAN L R.Analysis of selected herbicide metabolites in surface and ground water of the United States[J].Science of the total environment,2000,248(2):157-167.
[14]赵玲.二氧化锰体系下氯酚的非生物转化研究[D].广州:中国科学院(广州地球化学研究所),2006.
[15]RUBERT K F,PEDERSEN J A.Kinetics of oxytetracycline reaction with a hydrous manganese oxide[J].Environmental science&technology,2006,40(23):7216-7221.
[16]SHINDO H,HUANG P M.Significance of Mn(IV)oxide in abiotic formation of organic nitrogen complexes in natural environments[J].Nature,1984,308(5954):57-58.
[17]JIANG L Y,HUANG C,CHEN J M,et al.Oxidative transformation of 17β-estradiol by MnO2in aqueous solution[J].Archives of environmental contamination&toxicology,2009,57(2):221-229.
[18]ZHANG H,HUANG C H.Oxidative transformation of triclosan and chlorophene by manganese oxides[J].Environmental science&technology,2003,37(11):2421-2430.
[19]JIN Y S,CHENEY M A.Abiotic transformation of atrazine in aqueous suspension of four synthetic manganese oxides[J].Colloids&surfaces a physicochemical&engineering aspects,2004,242(1/2/3):85-92.
[20]BALDWIN D S,AND J K B,COLEMAN L M,et al.Hydrolysis of an organophosphate ester by manganese dioxide[J].Environmental science&technology,2001,35(4):713-716.
[21]LAHA S,LUTHY R G.Oxidation of aniline and other primary aromatic amines by manganese dioxide[J].Environmental science&technology,1990,24,3(3):363-373.
[22]MURRAY J W.The surface chemistry of hydrous manganese dioxide[J].Journal of colloid and interface science,1974,46(3):357-371.
[23]CHEN G,ZHAO L,DONG Y H.Oxidative degradation kinetics and products of chlortetracycline by manganese dioxide[J].Journal of hazardous materials,2011,193(20):128-138.
[24]KLAUSEN J,AND S B H,SCHWARZENBACH R P.Oxidation of substituted anilines by aqueous MnO2:effect of cosolutes on initial and quasi-steady-state kinetics[J].Environmental science&technology,1997,31(9):2642-2649.
[25]GAO J,PEDERSEN J A.Adsorption of sulfonamide antimicrobial agents to clay minerals[J].Environmental science&technology,2005,39(24):9509-9516.
[26]PAROLO M E,SAVINI M C,VALLS J M,et al.Tetracycline adsorption on montmorillonite:pH and ionic strength effects[J].Applied clay science,2008,40(1/2/3/4):179-186.
[27]FORREZ I,CARBALLA M,VERBEKEN K,et al.Diclofenac oxidation by biogenic manganese oxides[J].Environmental science&technology,2010,44(9):3449-3454.
[28]CHEN W R,HUANG C H.Transformation kinetics and pathways of tetracycline antibiotics with manganese oxide[J].Environmental pollution,2011,159(5):1092-1100.
[29]刘涉江,李木金,姜斌,等.甲基叔丁基醚(MTBE)在不同粘性土壤中的吸附特性[J].环境工程学报,2007,1(1):110-112.
[30]KOSMULSKI M.The pH-dependent surface charging and the points of zero charge[J].Journal of colloid&interface science,2002,253(1):77-87.
[31]FORREZ I,CARBALLA M,NOPPE H,et al.Influence of manganese and ammonium oxidation on the removal of 17alpha-ethinylestradiol(EE2)[J].Water research,2009,43(1):77-86.
[32]BARRETT K A,MCBRIDE M B.Oxidative degradation of glyphosate and aminomethylphosphonate by manganese oxide[J].Environmental science&technology,2005,39(23):9223-9228.
[33]STONE A T,MORGAN J J.Reduction and dissolution of manganese(III)and manganese(IV)oxides by organics.1.reaction with hydroquinone[J].Environmental science&technology,1984,18(6):450-456.