短裸甲藻对四种邻苯二甲酸酯的吸附降解研究
|
摘要
增塑剂是一种广泛存在于环境中的化学材料。邻苯二甲酸酯(Phthalic acid esters,简称PAEs)是增塑剂的主要种类,且易通过浸出、蒸发等迁移途径被释放到环境中,对环境造成污染。本研究选取了在海洋中广泛分布的典型藻类—短裸甲藻(Gymnodinium breve)作为受试生物。系统地比较了短裸甲藻对邻苯二甲酸二甲酯(Dimethyl phthalate,简称DMP)、邻苯二甲酸二乙酯(Diethyl phthalate,简称DEP)、邻苯二甲酸二烯丙酯(Diallyl phthalate,简称DAP)、邻苯二甲酸二丙酯(Dipropyl phtalate,简称DPr P)四种不同烷基链长度的PAEs的吸附降解情况。结果表明,PAEs烷基链越长,对短裸甲藻的生长抑制作用越强;藻液中PAEs浓度明显低于海水中PAEs浓度,证明藻类可以显著减少海水中的PAEs含量;与低藻密度的藻培养体系相比,高藻密度体系对溶解态的PAEs去除能力更强;高藻密度的藻体富集PAEs能力较强,但是平均到每个藻细胞,其富集能力远不如低藻密度的藻体;高藻密度的短裸甲藻对4种PAEs的降解能力如下:DMP(92.8%)>DEP(66.0%)>DAP(53.1%)>DPr P(42.6%)。本研究探讨了PAEs在藻培养体系中的降解过程,为PAEs在水环境中的消除奠定理论基础。
Plasticizers are a variety of chemicals which widely exist in the environment. Phthalic acid esters( PAEs) are the most important members and they can probably be transferred into the environment by exudation and vaporization processes,etc. And PAEs can become environmental pollutants. Gymnodinium breve,a species which is widely distributed around the world,is selected in this research to adsorb and degrade four kinds of PAEs: Dimethyl phthalate( DMP),Diethyl phthalate( DEP),Diallyl phthalate( DAP) and Dipropyl phtalate( DPr P). The results showed that PAE with longer alkyl chain exhibited more efficiency in depressing algae's growth. The concentrations of PAEs in solution became obviously lower than those in the seawater,demonstrating that algae could significantly decrease PAEs concentrations. Compared to lower-dense algae systems,higher-dense algae systems were more efficient in reducing PAEs concentrations. Algae cells in high-dense systems altogether absorbed more PAEs than those in low-dense systems,but the individuals in the later over-performed those in the former. The abilities to degrade different PAEs were listed in descending order as follows: DMP( 92. 8%) > DEP( 66. 0%) >DAP( 53. 1%) >DPr P( 42. 6%). This research explored such degradation process in an algae cultural system to throw some light on PAEs' removal theory.
Plasticizers are a variety of chemicals which widely exist in the environment. Phthalic acid esters( PAEs) are the most important members and they can probably be transferred into the environment by exudation and vaporization processes,etc. And PAEs can become environmental pollutants. Gymnodinium breve,a species which is widely distributed around the world,is selected in this research to adsorb and degrade four kinds of PAEs: Dimethyl phthalate( DMP),Diethyl phthalate( DEP),Diallyl phthalate( DAP) and Dipropyl phtalate( DPr P). The results showed that PAE with longer alkyl chain exhibited more efficiency in depressing algae's growth. The concentrations of PAEs in solution became obviously lower than those in the seawater,demonstrating that algae could significantly decrease PAEs concentrations. Compared to lower-dense algae systems,higher-dense algae systems were more efficient in reducing PAEs concentrations. Algae cells in high-dense systems altogether absorbed more PAEs than those in low-dense systems,but the individuals in the later over-performed those in the former. The abilities to degrade different PAEs were listed in descending order as follows: DMP( 92. 8%) > DEP( 66. 0%) >DAP( 53. 1%) >DPr P( 42. 6%). This research explored such degradation process in an algae cultural system to throw some light on PAEs' removal theory.
引文
[1]周庆祥,江桂斌.浅谈环境内分泌干扰物质[J].中国科技术语,2001,1(3):12-14.
[2]刘征涛.环境内分泌干扰效应与内分泌干扰素[J].中国科技术语,2001,3(3):15-16.
[3]李蕾,宋乃宁,李海山,等.邻苯二甲酸酯类毒理学效应及其机制研究进展[J].中国药理学与毒理学杂志,2014,28(3):468-474.
[4]Larsen S T,Hansen E W,et al.Airway inflammation and adjuvant effect after repeated airborne exposures to di-(2-ethylhexyl)phthalate and ovalbumin in BALB/c mice[J].Toxicology,2007,235(1):119-129.
[5]Saillenfait A M,Gallissot,Sabate J P.Differential developmental toxicities of di-n-hexyl phthalate and dicyclohexyl phthalate administered orally to rats[J].Journal of applied toxicology,2009,29(6):510-521.
[6]Foster P.Disruption of reproductive development in male rat offspring following in utero exposure to phthalate esters[J].International journal of andrology,2006,29(1):140-147.
[7]Boonyaroj V,Chiemchaisri C,Chiemchaisri W,et al.Toxic organic micropollutants removal mechanisms in long-term operated membrane bioreactor treating municipal solid waste leachate[J].Bioresource technology,2012,113,174-180.
[8]Ferreira I D,DE Menezes C B A,DE Oliveira V M,et al.Slurry Phase Biological Treatment of Latosol Contaminated with Phthalates,Adipate,and Alcohols[J].Journal of Environmental Engineering,2014,141(1),04014046(1-11).
[9]Staples C A,Peterson D R,Parkerton T F,et al.The environmental fate of phthalate esters:a literature review[J].Chemosphere,1997,35(4):667-749.
[10]Fromme H,Kuchler T,OTTO T,et al.Occurrence of phthalates and bisphenol A and F in the environment[J].Water research,2002,36(6):1429-1438.
[11]Rudel R A,Perovich L J.Endocrine disrupting chemicals in indoor and outdoor air[J].Atmospheric Environment,2009,43(1):170-181.
[12]Gomes R L,Scrimshaw M D,Lester J N.Determination of endocrine disrupters in sewage treatment and receiving waters[J].Tr AC Trends in Analytical Chemistry,2003,22(10):697-707.
[13]Birkett J W.Sources of endocrine disrupters[J].Endocrine Disrupters in Wastewater and Sludge Treatment Processes,2003:35-58.
[14]Liu X,Shi J,BO T,et al.Occurrence of phthalic acid esters in source waters:a nationwide survey in China during the period of 2009-2012[J].Environmental Pollution,2014(184):262-270.
[15]Mackintosh C E,Maldonado J,Hongwu J,et al.Distribution of phthalate esters in a marine aquatic food web:Comparison to polychlorinated biphenyls[J].Environmental Science&Technology,2004,38(7):2011-2020.
[16]Turner A,Rawling M C.The behaviour of di-(2-ethylhexyl)phthalate in estuaries[J].Marine Chemistry,2000,68(3):203-217.
[17]Heudorf U,Mersch-Sundermann V,Angerer J.Phthalates:toxicology and exposure[J].International journal of hygiene and environmental health,2007,210(5):623-634.
[18]方程冉.生物反应器填埋场中PAEs的迁移转化及其生物降解机制研究[D].浙江大学,2010.
[19]Sohoni P,Sumpter J P.Several environmental oestrogens are also anti-androgens[J].Journal of endocrinology,1998,158(3):327-339.
[20]张蕴晖.邻苯二甲酸二乙基已酯对环境和生物体的危害[J].环境卫生学杂志,2002,29(2):73-77.
[21]Magdouli S,Daghrir R,Brar S K,et al.Di 2-ethylhexyl phtalate in the aquatic and terrestrial environment:A critical review[J].Journal of environmental management,2013(127):36-49.
[22]孙翠竹,李富云,涂海峰,等.邻苯二甲酸酯类对水生食物链的影响研究进展[J].生态毒理学报,2016,11(6):12-24.
[23]况琪军,赵文玉,邓萍.DBP对斜生栅藻及天然混合藻类致毒效应研究[J].水生生物学报,2003,27(1):103-105.
[24]胡芹芹,熊丽,田裴秀子,等.邻苯二甲酸二丁酯(DBP)对斜生栅藻的致毒效应研究[J].生态毒理学报,2008,3(1):87-92.
[25]赫冬梅,钱晓佳,段舜山.邻苯二甲酸酯联合暴露对杜氏盐藻生长的影响[J].生态科学,2012,31(2):202-205.
[26]张化俊,彭云,张夙,等.溶藻细菌BS01产二异丁氧基苯基对塔玛亚历山大藻生长的影响[J].微生物学报,2015,55(7):834-842.
[27]阎海,雷志芳,叶常明.斜生栅藻降解邻苯二甲酸二甲酯和苯胺的动力学研究[J].环境科学学报,1998,18(2):216-219.
[28]Klekner V,Kosaric N.Degradation of phenols by algae[J].Environmental Technology Letters,1992,13(5):493-501.
[29]赵丽,刘征涛,冯流,等.单歧藻降解4-乙基酚的动力学研究[J].环境科学研究,2003,16(6):19-22.
[30]尤民生,刘新.农药污染的生物降解与生物修复[J].生态学杂志,2004,23(1):73-77.
[31]林毅雄.莱因衣藻(chlamgdomonas reinhardi Dang)和小球藻(Chlorella vulgaris Beij)对丙体-666的富集和降解的研究[J].中国环境科学,1984,4(2):15-21.
[32]Jinqi L,Houtian L.Degradation of azo dyes by algae[J].Environmental pollution,1992,75(3):273-278.
[33]刘厚田,杜晓明,刘金齐,等.藻菌系统降解偶氮染料的机理研究[J].环境科学学报,1993,13(3):332-338.
[34]邓星明,詹发萃,邓亚农.一种降解石油烃的淡水藻类—坑形席藻[J].植物学报,1982,24(6):548-553.
[35]Babu B,Wu J T.Biodegradation of phthalate esters by cyanobacterial[J].Journal of phycology,2010,46(6):1106-1113.
[36]Wolfe N L,Steen W C,Burns L A.Phthalate ester hydrolysis:linear free energy relationships[J].Chemosphere,1980,9(7):403-408.
[37]Roslev P,Vorkamp K,Aarup J,et al.Degradation of phthalate esters in an activated sludge wastewater treatment plant[J].Water Research,2007,41(5):969-976.
[38]Fang C,Long Y,Shen D.Removal of dibutyl phthalate from refuse from different phases of landfill in the presence of its dominant bacterial strains[J].Ecological Engineering,2014(71):87-93.
[39]Chang B V,Yang C M,Cheng C H,et al.Biodegradation of phthalate esters by two bacteria strains[J].Chemosphere,2004,55(4):533-538.
[40]王莹莹,范延臻,顾继东.邻苯二甲酸及邻苯二甲酸二甲酯的好氧微生物降解[J].应用与环境生物学报,2003,9(1):63-66.
[41]Gao,Chi J.Biodegradation of phthalate acid esters by different marine microalgal species[J].Marine pollution bulletin,2015,99(1-2):70-75.
[42]Guillard R R L,Ryther J H.Studies of marine planktonic diatoms:I.Cyclotella Nana Hustedt,and Detonula Confervacea(CLEVE)Gran[J].Canadian journal of microbiology,1962,8(2):229-239.
[43]Li F,Liang Z,Zheng X,et al.Toxicity of nano-Ti O 2 on algae and the site of reactive oxygen species production[J].Aquatic Toxicology,2015(158):1-13.
[44]黄丽雪.三种邻苯类增塑剂液相色谱检测条件的建立及应用[D].内蒙古农业大学,2012.
[45]卢伦.生物炭对水中邻苯二甲酸二乙酯的吸附研究[D].中国海洋大学,2015.
[46]王晶晶,钱晓佳,安民,等.邻苯二甲酸二乙酯和壬基酚联合暴露对杜氏盐藻生长的影响[J].生态科学,2012,31(4):370-376.
[47]吴志辉,聂湘平,杨宇峰,等.邻苯二甲酸二甲酯(DMP)对海洋微藻的生态毒理研究[J].生态科学,2006,25(2):168-170.
[48]田斐,何宁,段舜山.三种环境激素对四种海洋微藻的急性毒性效应研究[J].生态科学,2013,32(4):401-407.
[49]别聪聪,李锋民,李媛媛,等.邻苯二甲酸二丁酯对短裸甲藻活性氧自由基的影响[J].环境科学,2012,33(2):442-447.
[50]Liu N,Wen F L,LI F M,et al.Inhibitory mechanism of phthalate esters on Karenia brevis[J].Chemosphere,2016(155):498-508.
[51]Li F M,Wu M,Yao Y,et al.Inhibitory effects and oxidative target site of dibutyl phthalate on Karenia brevis[J].Chemosphere,2015(132):32-39.
[52]Rivera-Utrilla J,Ocampo-Perez R,Mendez-Diaz J D,et al.Environmental impact of phthalic acid esters and their removal from water and sediments by different technologies–a review[J].Journal of environmental management,2012,109(2012):164-178.
[53]Chan S M N,Luan T,Wong M H,et al.Removal and biodegradation of polycyclic aromatic hydrocarbons by Selenastrum capricornutum[J].Environmental toxicology and chemistry,2010,25(7):1772-1779.
[54]Liang D W,Zhang T,Fang H H,et al.Phthalates biodegradation in the environment[J].Applied microbiology and Biotechnology,2008,80(2):183.
[55]Gao Q T,Wong Y S,Tam N F Y.Removal and biodegradation of nonylphenol by different Chlorella species[J].Marine pollution bulletin,2011,63(5-12):445-451.
[56]李媛媛.化感物质对短裸甲藻产生毒素的影响[D].中国海洋大学,2012.
[57]Li Y,Gao J,Meng F,et al.Enhanced biodegradation of phthalate acid esters in marine sediments by benthic diatom Cylindrotheca closterium[J].Science of The Total Environment,2015,508(508C):251-257.
[2]刘征涛.环境内分泌干扰效应与内分泌干扰素[J].中国科技术语,2001,3(3):15-16.
[3]李蕾,宋乃宁,李海山,等.邻苯二甲酸酯类毒理学效应及其机制研究进展[J].中国药理学与毒理学杂志,2014,28(3):468-474.
[4]Larsen S T,Hansen E W,et al.Airway inflammation and adjuvant effect after repeated airborne exposures to di-(2-ethylhexyl)phthalate and ovalbumin in BALB/c mice[J].Toxicology,2007,235(1):119-129.
[5]Saillenfait A M,Gallissot,Sabate J P.Differential developmental toxicities of di-n-hexyl phthalate and dicyclohexyl phthalate administered orally to rats[J].Journal of applied toxicology,2009,29(6):510-521.
[6]Foster P.Disruption of reproductive development in male rat offspring following in utero exposure to phthalate esters[J].International journal of andrology,2006,29(1):140-147.
[7]Boonyaroj V,Chiemchaisri C,Chiemchaisri W,et al.Toxic organic micropollutants removal mechanisms in long-term operated membrane bioreactor treating municipal solid waste leachate[J].Bioresource technology,2012,113,174-180.
[8]Ferreira I D,DE Menezes C B A,DE Oliveira V M,et al.Slurry Phase Biological Treatment of Latosol Contaminated with Phthalates,Adipate,and Alcohols[J].Journal of Environmental Engineering,2014,141(1),04014046(1-11).
[9]Staples C A,Peterson D R,Parkerton T F,et al.The environmental fate of phthalate esters:a literature review[J].Chemosphere,1997,35(4):667-749.
[10]Fromme H,Kuchler T,OTTO T,et al.Occurrence of phthalates and bisphenol A and F in the environment[J].Water research,2002,36(6):1429-1438.
[11]Rudel R A,Perovich L J.Endocrine disrupting chemicals in indoor and outdoor air[J].Atmospheric Environment,2009,43(1):170-181.
[12]Gomes R L,Scrimshaw M D,Lester J N.Determination of endocrine disrupters in sewage treatment and receiving waters[J].Tr AC Trends in Analytical Chemistry,2003,22(10):697-707.
[13]Birkett J W.Sources of endocrine disrupters[J].Endocrine Disrupters in Wastewater and Sludge Treatment Processes,2003:35-58.
[14]Liu X,Shi J,BO T,et al.Occurrence of phthalic acid esters in source waters:a nationwide survey in China during the period of 2009-2012[J].Environmental Pollution,2014(184):262-270.
[15]Mackintosh C E,Maldonado J,Hongwu J,et al.Distribution of phthalate esters in a marine aquatic food web:Comparison to polychlorinated biphenyls[J].Environmental Science&Technology,2004,38(7):2011-2020.
[16]Turner A,Rawling M C.The behaviour of di-(2-ethylhexyl)phthalate in estuaries[J].Marine Chemistry,2000,68(3):203-217.
[17]Heudorf U,Mersch-Sundermann V,Angerer J.Phthalates:toxicology and exposure[J].International journal of hygiene and environmental health,2007,210(5):623-634.
[18]方程冉.生物反应器填埋场中PAEs的迁移转化及其生物降解机制研究[D].浙江大学,2010.
[19]Sohoni P,Sumpter J P.Several environmental oestrogens are also anti-androgens[J].Journal of endocrinology,1998,158(3):327-339.
[20]张蕴晖.邻苯二甲酸二乙基已酯对环境和生物体的危害[J].环境卫生学杂志,2002,29(2):73-77.
[21]Magdouli S,Daghrir R,Brar S K,et al.Di 2-ethylhexyl phtalate in the aquatic and terrestrial environment:A critical review[J].Journal of environmental management,2013(127):36-49.
[22]孙翠竹,李富云,涂海峰,等.邻苯二甲酸酯类对水生食物链的影响研究进展[J].生态毒理学报,2016,11(6):12-24.
[23]况琪军,赵文玉,邓萍.DBP对斜生栅藻及天然混合藻类致毒效应研究[J].水生生物学报,2003,27(1):103-105.
[24]胡芹芹,熊丽,田裴秀子,等.邻苯二甲酸二丁酯(DBP)对斜生栅藻的致毒效应研究[J].生态毒理学报,2008,3(1):87-92.
[25]赫冬梅,钱晓佳,段舜山.邻苯二甲酸酯联合暴露对杜氏盐藻生长的影响[J].生态科学,2012,31(2):202-205.
[26]张化俊,彭云,张夙,等.溶藻细菌BS01产二异丁氧基苯基对塔玛亚历山大藻生长的影响[J].微生物学报,2015,55(7):834-842.
[27]阎海,雷志芳,叶常明.斜生栅藻降解邻苯二甲酸二甲酯和苯胺的动力学研究[J].环境科学学报,1998,18(2):216-219.
[28]Klekner V,Kosaric N.Degradation of phenols by algae[J].Environmental Technology Letters,1992,13(5):493-501.
[29]赵丽,刘征涛,冯流,等.单歧藻降解4-乙基酚的动力学研究[J].环境科学研究,2003,16(6):19-22.
[30]尤民生,刘新.农药污染的生物降解与生物修复[J].生态学杂志,2004,23(1):73-77.
[31]林毅雄.莱因衣藻(chlamgdomonas reinhardi Dang)和小球藻(Chlorella vulgaris Beij)对丙体-666的富集和降解的研究[J].中国环境科学,1984,4(2):15-21.
[32]Jinqi L,Houtian L.Degradation of azo dyes by algae[J].Environmental pollution,1992,75(3):273-278.
[33]刘厚田,杜晓明,刘金齐,等.藻菌系统降解偶氮染料的机理研究[J].环境科学学报,1993,13(3):332-338.
[34]邓星明,詹发萃,邓亚农.一种降解石油烃的淡水藻类—坑形席藻[J].植物学报,1982,24(6):548-553.
[35]Babu B,Wu J T.Biodegradation of phthalate esters by cyanobacterial[J].Journal of phycology,2010,46(6):1106-1113.
[36]Wolfe N L,Steen W C,Burns L A.Phthalate ester hydrolysis:linear free energy relationships[J].Chemosphere,1980,9(7):403-408.
[37]Roslev P,Vorkamp K,Aarup J,et al.Degradation of phthalate esters in an activated sludge wastewater treatment plant[J].Water Research,2007,41(5):969-976.
[38]Fang C,Long Y,Shen D.Removal of dibutyl phthalate from refuse from different phases of landfill in the presence of its dominant bacterial strains[J].Ecological Engineering,2014(71):87-93.
[39]Chang B V,Yang C M,Cheng C H,et al.Biodegradation of phthalate esters by two bacteria strains[J].Chemosphere,2004,55(4):533-538.
[40]王莹莹,范延臻,顾继东.邻苯二甲酸及邻苯二甲酸二甲酯的好氧微生物降解[J].应用与环境生物学报,2003,9(1):63-66.
[41]Gao,Chi J.Biodegradation of phthalate acid esters by different marine microalgal species[J].Marine pollution bulletin,2015,99(1-2):70-75.
[42]Guillard R R L,Ryther J H.Studies of marine planktonic diatoms:I.Cyclotella Nana Hustedt,and Detonula Confervacea(CLEVE)Gran[J].Canadian journal of microbiology,1962,8(2):229-239.
[43]Li F,Liang Z,Zheng X,et al.Toxicity of nano-Ti O 2 on algae and the site of reactive oxygen species production[J].Aquatic Toxicology,2015(158):1-13.
[44]黄丽雪.三种邻苯类增塑剂液相色谱检测条件的建立及应用[D].内蒙古农业大学,2012.
[45]卢伦.生物炭对水中邻苯二甲酸二乙酯的吸附研究[D].中国海洋大学,2015.
[46]王晶晶,钱晓佳,安民,等.邻苯二甲酸二乙酯和壬基酚联合暴露对杜氏盐藻生长的影响[J].生态科学,2012,31(4):370-376.
[47]吴志辉,聂湘平,杨宇峰,等.邻苯二甲酸二甲酯(DMP)对海洋微藻的生态毒理研究[J].生态科学,2006,25(2):168-170.
[48]田斐,何宁,段舜山.三种环境激素对四种海洋微藻的急性毒性效应研究[J].生态科学,2013,32(4):401-407.
[49]别聪聪,李锋民,李媛媛,等.邻苯二甲酸二丁酯对短裸甲藻活性氧自由基的影响[J].环境科学,2012,33(2):442-447.
[50]Liu N,Wen F L,LI F M,et al.Inhibitory mechanism of phthalate esters on Karenia brevis[J].Chemosphere,2016(155):498-508.
[51]Li F M,Wu M,Yao Y,et al.Inhibitory effects and oxidative target site of dibutyl phthalate on Karenia brevis[J].Chemosphere,2015(132):32-39.
[52]Rivera-Utrilla J,Ocampo-Perez R,Mendez-Diaz J D,et al.Environmental impact of phthalic acid esters and their removal from water and sediments by different technologies–a review[J].Journal of environmental management,2012,109(2012):164-178.
[53]Chan S M N,Luan T,Wong M H,et al.Removal and biodegradation of polycyclic aromatic hydrocarbons by Selenastrum capricornutum[J].Environmental toxicology and chemistry,2010,25(7):1772-1779.
[54]Liang D W,Zhang T,Fang H H,et al.Phthalates biodegradation in the environment[J].Applied microbiology and Biotechnology,2008,80(2):183.
[55]Gao Q T,Wong Y S,Tam N F Y.Removal and biodegradation of nonylphenol by different Chlorella species[J].Marine pollution bulletin,2011,63(5-12):445-451.
[56]李媛媛.化感物质对短裸甲藻产生毒素的影响[D].中国海洋大学,2012.
[57]Li Y,Gao J,Meng F,et al.Enhanced biodegradation of phthalate acid esters in marine sediments by benthic diatom Cylindrotheca closterium[J].Science of The Total Environment,2015,508(508C):251-257.