胶体迁移及其对典型类固醇雌激素的吸附
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摘要
研究胶体自身的可迁移性和对污染物的可吸附性能够为地下环境中胶体对污染物的携带迁移作用提供重要依据。通过动态柱实验和静态批实验研究二氧化硅胶体、伊利石胶体和胡敏酸胶体在饱和多孔介质中的可迁移性以及对雌酮和雌二醇的吸附作用。结果表明:不同胶体在饱和多孔介质中的可迁移性有所差异,胡敏酸胶体和二氧化硅胶体分别在石英砂柱和河砂砂柱中迁移性最强,而伊利石胶体在2种多孔介质中的迁移性均较弱;准二级动力学模型对胶体吸附雌激素的数据拟合效果最好,吸附速率的控制因素可能包括表面吸附、化学络合等;Langmuir模型对胶体吸附雌激素的拟合效果较Freundlich模型更好,推测胶体对雌激素的吸附为单层吸附,3种胶体对雌酮和雌二醇的最大吸附量分别为90.09～3 333 mg?kg~(-1)和116.28～2 000 mg?kg~(-1)。因此,胶体的可迁移性和对雌激素的吸附作用能够为胶体影响雌激素在地下环境中的迁移提供理论指导。
The study of colloids mobility and their adsorption of contaminants may provide an important basis for the carrying and migration of contaminants by colloids in subsurface environment. The mobility of silica colloids, illite colloids and humic acid(HA) colloids through saturated porous medium and their adsorption of estrone(E1) and estradiol(E2) were studied through dynamic column and static batch experiments. The results showed that there was significant difference in the migration properties among the three types of colloids in saturated porous media. HA and silica colloid presented the highest mobility in the quartz sand column and the river sand column, respectively, while illite colloid had poor migration performances in both porous media. The pseudo-second order kinetic model provides the best fitting for the data of estrogens adsorption on colloids.Surface adsorption and chemical complexation may be the control factors of adsorption rate. The estrogen adsorption isotherms on colloids could be better fitted by Langmuir model than Freundlich model, which may indicate that the monolayer adsorption of estrogen occurred on colloids. The maximum adsorption capacities of estrone and estradiol on colloids were 90.09～3 333 mg?kg~(-1) and 116.28～2 000 mg?kg~(-1), respectively. Therefore,colloidal mobility and their adsorption of typical steroid estrogens can provide theoretical guidance for the effect of colloids on estrogens migration in subsurface environment.
The study of colloids mobility and their adsorption of contaminants may provide an important basis for the carrying and migration of contaminants by colloids in subsurface environment. The mobility of silica colloids, illite colloids and humic acid(HA) colloids through saturated porous medium and their adsorption of estrone(E1) and estradiol(E2) were studied through dynamic column and static batch experiments. The results showed that there was significant difference in the migration properties among the three types of colloids in saturated porous media. HA and silica colloid presented the highest mobility in the quartz sand column and the river sand column, respectively, while illite colloid had poor migration performances in both porous media. The pseudo-second order kinetic model provides the best fitting for the data of estrogens adsorption on colloids.Surface adsorption and chemical complexation may be the control factors of adsorption rate. The estrogen adsorption isotherms on colloids could be better fitted by Langmuir model than Freundlich model, which may indicate that the monolayer adsorption of estrogen occurred on colloids. The maximum adsorption capacities of estrone and estradiol on colloids were 90.09～3 333 mg?kg~(-1) and 116.28～2 000 mg?kg~(-1), respectively. Therefore,colloidal mobility and their adsorption of typical steroid estrogens can provide theoretical guidance for the effect of colloids on estrogens migration in subsurface environment.
引文
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[20]王博,李海明,贾晓玉,等.天然胶体对含水介质中氨氮迁移的影响[J].环境科学与技术, 2009, 32(7):18-21.
[21]胡俊栋,沈亚婷,王学军.土壤胶体在不同饱和度土壤介质中的释放与淋溶行为研究[J].农业环境科学学报, 2009, 28(9):1829-1836.
[22]王园园,宋晓明,温玉娟,等.固相萃取-衍生化-气相色谱-质谱联用测定不同水体中类固醇雌激素方法研究[J].岩矿测试, 2017, 36(5):519-528.
[23] ANDERSEN H R, HANSEN M, KJOLHOLT J, et al. Assessment of the importance of sorption for steroid estrogens removal during activated sludge treatment[J]. Chemosphere, 2005, 61(1):139-146.
[24] WANG H, LIU Y G, ZENG G M, et al. Grafting ofβ-cyclodextrin to magnetic graphene oxide via ethylenediamine and application for Cr(VI)removal[J]. Carbohydrate Polymers, 2014, 113:166-173.
[25]杨悦锁,王园园,宋晓明,等.土壤和地下水环境中胶体与污染物共迁移研究进展[J].化工学报, 2017, 68(1):23-36.
[26] LIMA D L, CALISTO V, ESTEVES V I. Adsorption behavior of 17β-ethynylestradiol onto soils followed by fluorescence spectral deconvolution[J]. Chemosphere, 2011, 84(8):1072-1078.
[27] GAO P, FENG Y, ZHANG Z, et al. Comparison of competitive and synergetic adsorption of three phenolic compounds on river sediment[J]. Environmental Pollution, 2011, 159(10):2876-2881.
[28]齐瑞环,李兆君,龙健,等.土壤粉碎粒径对土霉素在土壤中吸附的影响[J].环境科学, 2011, 32(2):589-595.
[2] HIEMENZ P C, RAJAGOPALAN R. Principles of Colloid and Surface Chemistry[M]. 3rd Edition. New York:Marcel Dekker,1997.
[3] VIGNATI D, DOMINIK J. The role of coarse colloids as a carrier phase for trace metals in riverine systems[J]. Aquatic Science, 2003, 65(2):129-142.
[4] KRETZSCHMAR R, BORKOVEC M, GROLIMUND D, et al. Mobile subsurface colloid and their role in contaminant transport[J]. Advances in Agronomy, 1999, 66:121-193.
[5] SYNGOUNA V I, CHRYSIKOPOULOS C V. Co-transport of clay colloids and viruses in water saturated porous media[J].Colloids&Surfaces A:Physicochemical&Engineering Aspects, 2013, 416(1):56-65.
[6]金光球,李凌.河流中潜流交换研究进展[J].水科学进展, 2008, 19(2):285-293.
[7] SWARTZ C H, REDDY S, BENOTTI M J, et al. Steroid estrogens, nonylphenol ethoxylate metabolites, and other wastewater contaminants in groundwater affected by a residential septic system on Cape Cod, MA[J]. Environmental Science&Technology, 2006, 40(16):4894-4902.
[8]陈蕾,王郑,曹世玮.畜禽养殖排放的雌激素对周边水体环境的影响[J].生态环境学报, 2014, 23(2):359-364.
[9] CASEY F X M, LARSEN G L, HAKK H, et al. Fate and transport of 17β-estradiol in soil-water systems[J]. Environmental Science&Technology, 2003, 37:2400-2409.
[10] BOWMAN J C, ZHOU J L, READMAN J W. Sediment-water interactions of natural oestrogens under estuarine conditions[J].Marine Chemistry, 2002, 77:263-276.
[11] LEE L S, STROCK T J, SARMAH A K, et al. Sorption and dissipation of testosterone, and estrogens, and their primar transformation products in soils and sediments[J]. Environmental Science&Technology, 2003, 37:4098-4105.
[12] TAO C, JAMES E S. Colloid-facilitated transport of cesium in vadose-zone sediments:The importance of flow transients[J].Environmental Science&Technology, 2010, 44:7443-7449.
[13] DANIEL G. Colloid-facilitated transport of strongly sorbing contaminants in natural porous media:Mathematical modeling and laboratory column experiments[J]. Environmental Science&Technology, 2005, 39:6378-6386.
[14] YAN C X, NIE M H, YI Y. Effect of colloids on the occurrence, distribution and photolysis of emerging organic contaminants in wastewaters[J]. Journal of Hazardous Materials, 2015, 299:241-248.
[15] SEETHA N, MOHAN K M S, HASSANIZADEH S M. Modeling the co-transport of viruses and colloids in unsaturated porous media[J]. Journal of Contaminant Hydrology, 2015, 181:82-101.
[16] BRADFORD S A, SIMUNEK J, BETTAHAR M, et al. Modeling colloid attachment, straining, and exclusion in saturated porous media[J]. Environmental Science&Technology, 2003, 37:2242-2250.
[17] KELLER A A, AUSET M. A review of visualization techniques of biocolloid transport processes at the pore scale under saturated and unsaturated conditions[J]. Advances in Water Resources, 2007, 30:1392-1407.
[18]靳青,张增强,岳波,等. 17α-雌二醇在土壤样品中的吸附特性研究[J].环境工程, 2012, 30(4):121-126.
[19]陈斌,马伟芳,曾凡刚,等.类固醇雌激素在土壤与沉积物中的污染水平及其吸附研究进展[J].环境工程, 2014, 32(7):131-137.
[20]王博,李海明,贾晓玉,等.天然胶体对含水介质中氨氮迁移的影响[J].环境科学与技术, 2009, 32(7):18-21.
[21]胡俊栋,沈亚婷,王学军.土壤胶体在不同饱和度土壤介质中的释放与淋溶行为研究[J].农业环境科学学报, 2009, 28(9):1829-1836.
[22]王园园,宋晓明,温玉娟,等.固相萃取-衍生化-气相色谱-质谱联用测定不同水体中类固醇雌激素方法研究[J].岩矿测试, 2017, 36(5):519-528.
[23] ANDERSEN H R, HANSEN M, KJOLHOLT J, et al. Assessment of the importance of sorption for steroid estrogens removal during activated sludge treatment[J]. Chemosphere, 2005, 61(1):139-146.
[24] WANG H, LIU Y G, ZENG G M, et al. Grafting ofβ-cyclodextrin to magnetic graphene oxide via ethylenediamine and application for Cr(VI)removal[J]. Carbohydrate Polymers, 2014, 113:166-173.
[25]杨悦锁,王园园,宋晓明,等.土壤和地下水环境中胶体与污染物共迁移研究进展[J].化工学报, 2017, 68(1):23-36.
[26] LIMA D L, CALISTO V, ESTEVES V I. Adsorption behavior of 17β-ethynylestradiol onto soils followed by fluorescence spectral deconvolution[J]. Chemosphere, 2011, 84(8):1072-1078.
[27] GAO P, FENG Y, ZHANG Z, et al. Comparison of competitive and synergetic adsorption of three phenolic compounds on river sediment[J]. Environmental Pollution, 2011, 159(10):2876-2881.
[28]齐瑞环,李兆君,龙健,等.土壤粉碎粒径对土霉素在土壤中吸附的影响[J].环境科学, 2011, 32(2):589-595.