土壤/沉积物对挥发性有机污染物的吸附研究
详细信息    本馆镜像全文|  推荐本文 |  |   获取CNKI官网全文
摘要
近年来,土壤/沉积物污染的状况日趋严重。就污染的种类、污染的范围以及对生物有机体的危害,有机污染排在所有污染的首位。本文就土壤/沉积物对挥发性有机污染物的吸附行为特征进行了系统的研究,选用污染最广泛、具有代表性的2种挥发性有机污染物,定性定量地研究不同地区土壤的吸附特性,通过系统分析检测土壤自身物理特性,深入研究了土壤自身特性对有机污染物的吸附规律。主要结论如下:
    土样颗粒分布与吸附行为没有明显的相关关系;有机碳总量foc和CEC与吸附存在较为明显的相关关系。其中foc和CEC存在较明显的线性相关关系,结果为CEC = 5.4563(foc) + 5.6051,R2 = 0.8921。
    石英砂和高岭土对目标污染物TCE和苯基本不存在吸附作用,或吸附作用极弱,不易体现。
    有机碳含量对土样吸附能力影响较大。3种高有机碳含量土样TCE和苯的吸附线均为线性,R2依次为0.9738~0.9910、0.9203~0.9967;3组低有机碳含量土样对TCE和苯的吸附在高浓度时吸附浓度增加缓慢,非线性明显,吸附方程用Langmuir式拟合相关性较好,R2依次为0.8982~0.9426、0.9228~0.9902。
    有机碳的聚合形式对TCE的吸附影响较小,对苯的吸附影响较大。一级土样和二级土样有机碳标准化后,对于TCE,logKoc均在2.086±0.168~2.274±0.169;对于苯,logKoc(一级土样)2.791±0.113~3.455±0.292,logKoc(二级土样)1.848±0.142~2.026±0.142。对于苯,含有“黑碳粒子”的低聚碳,表现出对苯更强的吸附能力。
    土壤总有机碳对TCE的吸附量,等于低聚碳和高聚碳吸附量之和。吸附实验体系中,苯吸附率在0.1%~80%,TCE吸附率在30%~70%;苯的液相存留率在0.1%~80%,TCE的液相存留率在30%~60%;苯的挥发率近1/5,TCE挥发率约1/3。
The soil (sediment) contamination is gradually serious in the last years. Organicchemicals in soils (sediments) are the first for the category and scope of contaminationand its harm to organism. This paper researches the sorption of the volatile Organicchemicals in soils, especially for TCE and Benzene. The sorption characteristic of soilitself is also researched in the numbers. The followings were the main results.
    The particle contents of soils was not correlative with the sorption, however thetotal organic carbon (foc) was correlative with the CEC, and the relation of foc andCEC was CEC = 5.4563(foc) + 5.6051,R2 = 0.8921.
    TCE and Benzene were hardly absorbed by the quartz and kaolinite.
    The sorption capacity of soils on TCE and Benzene was correlative with the organiccarbon of soils. Three surface soils with rich organic carbon ,the isotherms of TCE andBenzene were linear, R2 for TCE and Benzene were 0.9738~0.9910 and 0.9203~0.9967,while three underground water with poor organic carbon, the isotherms were nonlinear,which can be described with Langmuir equation, R2 for TCE and Benzenewere0.8982~0.9426、0.9228~0.9902.
    The structure of organic carbon was hardly inflected to the sorption on TCE,however it was evidently done to sorption on Benzene. The partition coefficient(normalized to organic carbon ) logKoc of the samples and sub-samples for TCE were all2.086±0.168~2.274±0.169, and for Benzene logKoc(sample soils) was 2.791±0.113~3.455±0.292,logKoc(sub-samples)was 1.848±0.142~2.026±0.142. The incompactblack carbon particle aggregation had more adsorbability to Benzene than to TCE.
    The total sorption capacities of organic carbon on TCE equal to the sorptioncapacities of incompact carbon aggregation and compact carbon aggregation.
    In the experiment systems, the sorption percents of Benzene were 0.1%~80% , andthese of TCE were 30%~70%. The percents in solution of Benzene were 0.1%~80%,however these of TCE were 30%~60%. The volatilization percents of Benzene were upto 20%, and these of TCE were also up to 33%.
引文
[1]武晓峰,唐杰,藤间幸久,有机污染在多孔介质中的残留,云南环境科学,第 19 卷,增刊,p46-49。
    [2]占伟,吴文忠等,有机有毒污染物在土壤及底泥系统中的吸附/解析行为研究进展,环境科学进展,1998 年,Vol.6,No.3,p1-11。
    [3]张立成,章申,董文江,赵桂久,湘江江水中重金属转化地球化学因素[j],环境科学学报,1986,6(4):395-402。
    [4]韩伟明,张国勋,杭州西湖底泥释磷的模拟研究[J]。In:西湖环境研究论文集,1990:83-89。
    [5]杨瑞强,非离子型有机污染物在黄土中的吸附行为,2002 年 6 月,西北师范大学,硕士学位论文
    [6] C.T. Chiou, L.J. Peters, and V.H. Freed, A physical concept of soil-water equilibrium for nonionic organic compounds. Science (Washington, DC). 206 (16) (1979) 831-832.
    [7]丁应详,朱琰,黄剑朎,有机污染在土壤-水体系中的分配理论,农村生态环境,1997,Vol.13, No.3,p42-45。
    [8]Chou CT, Schmedding D W. Partitioning of organic compounds in octanol-water systems. Environ Sci Technol. 1982, vol.16,p4-10。
    [9]Chou CT, Potter PE, Schmedding D W. Partition equilibria of nonionic organic compounds between soil organic matter and water. Environ Sci Technol. 1983, vol.17,p27-231。
    [10]王文华,王淑琴,徐维并,北京昆明湖底泥中有机物的表征[J],环境科学学报,1995,15(2):178-185。
    [11]Chiou CT, Malcolm RL, Brinton TI et al. Water solubility enhancement of some organic pollutants and pesticides by dissolved humic and fulvic acids. Environ Sci Technol.1988, Vol.22,p298-303。
    [12]Huang W, Schalutman M A, Weber W J Jr. Environ Sci Technol.1996, Vol.30,p2993-3000。
    [13]Moder B T, Uwe-Goos K, Eisenreich S J. Environ Sci Technol.1997, Vol.31,p1079-1086。
    [14] 南京农科所,土壤理化分析,[M],南京:
    [15] Lambert S M, Porter P E, Schieferstein R H. Weeds, 1965, Vol.13,p185-190。
    [16] MackayD, Bobra A, shiu W Y, et al. Chem osphere, 1980, Vol.9,p701-711。
    [17]Schwarzenbach R P, Westall J. Environ Sci Technol. 1981,Vol.15,p1360-1367。
    [18]Chiou C T, Poter P E, Schmedding D W. Environ Sci Technol., 1983,vol.17,p227-231。
    [19]Means J C, Wood S G, Hassett J J, et al. Environ Sci Technol. 1982,vol.16,No.2,p93-98。
    [20]党志,于虹,土壤/沉积物吸附有机污染物机理研究进展,化学通报,2001,vol.2,p81-85。
    [21]Mohsen Mehran, Roger L. Olsen and Bryan M.Rector. Distribution Coefficient of Trichloroethylene in Soil-water Systems, p275-282。
    [22]Weber W J Jr., McGinley P M, Katz L E. Environ. Sci Technol., 1992,Vol.26,p1956-1962。
    [23]Young T M, W J Jr. Environ. Sci Technol., 1995,Vol.29,p92-97。
    [24]Weber W J Jr., Huang W. Environ. Sci Technol., 1996,Vol.30,p881-888。
    [25]Huang W, Young T M, Schlautm M A, et al. Environ. Sci Technol., 1997,Vol.31,p1703-1710。
    [26]Blom,G,Winkels,H.J.Modeling sediment accumulation and dispersion of contaminants in lake Ijsselmeer(the Netherlands)[J].Wat.Sdi.Tech.,1998;37(6-7):17-24
    [27]Bremle G,Okla L,Larsson P.Upeake of PCBs infish in contaminatd river systems:bioconcentration factorsmeasured in field[J].Environ Sci Technol,1995,29;2010-2015
    [28]曲久辉。我国水体复合污染与控制[J].科学对社会的影响,2000;1:36-40
    [29]Stortelder P B M.Management of contaminated sediment,an overview[J]. European Water Pollution Control,1995;5(5):8-15
    [30]金相灿等。中国湖泊环境(第一册)[M].北京:海洋出版社,1995
    [31]高兴斋.湘江重金属污染特征.In:陈端生,黄玉凯,高兴斋,张玉清.河流重金属污染研究.北京:中国环境科学出版社,1987:69-79
    [32] US EPA.EPA's contaminated Sediment Management Strategy. EPA, 1998,823-R-98-001.
    [33] Yuan D, Yang D, Wade T L, Qian Y. Status of persistent organic pollutants in the sediment from several estuaries in China[J]. Environmental Pollution, 2001,114:101-111.
    [34] Kubicki J D, and Apita S E. Models of natural organic matter and interactions with organic contaminants [J]. Organic Geochemistry, 1999,30:911-927.
    [35] Xu S, Song Y, Sun C, Feng J, Wang L, Martes D, Gawlic B M. Polychlorinated organic compounds in Yangtes River sediments [J] Chemosphere, 2000,41:1897-1903.
    [36] Lee C L, song H J, and fang M D. Concentrations of chloro 苯 s, hexachlorobutadiene and heavy metals in surficial sediments of Kaohiung coast, Taiwan [J]. Chemosphere, 2000, 41:889-899.
    [37]LeBoeuf E J, Weber W J Jr. Environ. Sci Technol., 1997,Vol.31,p1697-1702。
    [38]Pignatello J J. Organic substances and sedments in water, Vol.2. Humics and soils. Chelsea, Michian: Lew is Publishers, 1991, p291-307。
    [39]Pignatello J J, Xing B. Environ. Sci Technol., 1996,Vol.30,p1-11。
    [40] Xing B, Pignatello J J, Gigliotti B. Environ. Sci Technol., 1996,Vol.30,p2432-2440。
    [41] Xing B, Pignatello J J. Environ. Toxicology and Chemistry, 1996, Vol.15, p1282-1288。
    [42]Hayes M B H, MacCarthy R M, et al. Humic substances Ⅱ:in search of structure, Hayes M B H, et al., Eds. New York:John Wiley and sons, 1989。
    [43]党志,黄伟林,肖保华,有机污染物-土壤/沉积物吸附作用研究,矿物岩石 地球化学通报,1999,vol.18, No.3,p194-196。
    [44]Bailey G W, White J L. Factors influencing the adsorption and movement of pesticides in soil. Residue Rev., 1970, Vol.32, p29-92。
    [45]Kanckhoff S W, Brown D S, Scott T A. Sorption of hydrophobic pollutants on naturee sediments. Water Res., 1979, Vol.13, 241-248。
    [46]Chiou C T , Peters L J, Freed V H. A physical concept of soil-water equilibria for nonionici organic compounds. Science, 1979, Vol.206, No.16, p831-832。
    [47]Means J C, Wood S G, Hassett J J et al. Sorption of polynuclear aromatic hydrocarbons by sediments and soils. Environ. Sci. Technol., 1980, Vol.14, No.12,p1524-1528。
    [48] Rene P. Schwarzenbach and John Weatall, Transport of Nonpolar Organic Compounds from surfaces water to groundwater: Laboratory sorption studies. Environ. Sci. Technol., 1981, Vol.15, No.11,p1360-1367。
    [49] 凌婉婷,徐建民,高彦征,汪海珍,溶解性有机质对土壤中有机污染物环境行为的影响,应用生态学报,2004 年,Vol.15, No.2, 326-330。
    [50] Fredeen F J H,Arnason A P, Berek B. Adsorption of DDT on suspended soils in river water and its role in black fly control. Nature Vol.171, p700-701。
    [51] William G. Maclntyre, Thomas B. Stauffer and Christopher P. Antworth, Ground Water , 1991,Vol.29, No.6, p908-913。
    [52] Gshwend P M, Wu S C. On the constancy of sediment water partition coefficients of hydrophobic organic pollutants. Environ. Sci. Technol., 1985, Vol.19, No.1,p90-96。
    [53]Loruival Costa Paraiba, Soil temperature effect in calculating attenuation and retardation factores. Chemosphere 48 (2002),905-912。
    [54]A.S.Abdul, T.L.Gibson, D.N.Rai, Laboratory studies of the flow some organic solvents and their aqueous solutions through bentonite and Kaolin Clays. Groundwater,1990,Vol.28, No.4,524-533.
    [55] William G. Maclntyre, Thomas B. Staurrer, Christopher P.antworth, A Comparison of sorption coefficients determined by batch, column, and bos methods on a low organic carbon aquifer material.groundwater, 1991,Vol.29,No.6,908-913.
    [56] Butterfield, Nicholas James,The sorption of nonionic organic solutes to humic acid-mineral complexes, Ph.D. dissertation,Harvard University,1992.
    [57] Tamara W. Sheremata, The influence of soil organic matter on the fate of trichloroethylene in soil, Ph.D. dissertation, McGill University,1997.
    [58] Arands, Rolf Roland, Sorption and diffusion of 苯, toluene, and the xylenes in unsaturated soil, Ph.D. dissertation, Rutgers The State University of New Jersey.New Brunswick,1994.
    [59] Baohua Xiao,The effects of soil organic matter heterogeneity on equilibrium sorption by soils and sediments, Ph.D. dissertation, Dresel Unisity, 2004.
    [60] M. Ghiaci , A. Abbaspur, R. Kia, F. Seyedeyn-Azad, Equilibrium isotherm studies for the sorption of 苯 , toluene, and phenol onto organo-zeolites and as-synthesized MCM-41, Separation and Purification Technology 40 (2004) 217–229
    [61] Vera W. Langer, Kent S. Novakowski , Allan D. Woodbury, Sorption of trichloroethene onto stylolites, _ . Journal of Contaminant Hydrology 40 1999 1–23
    [61] 唐常源,饱和粘土中的三氯乙烯迁移特性,应用生态学报,1997 年,Vol.7, No.1,94-98。
    [62] 魏玺群,陈健,吸附剂对三氯乙烯的吸附及解吸,低温与特气,1999 年,No.1.38-40.
    [63] 宁平,谷俊杰,H.J.Bart,田森林,低浓度三氯乙烯活性炭吸附净化及数值模拟,化学工程,2000 年,vol.28,no.1,35-38.
    [64] vol.28,no.1 沉积物化学浸取与毒性有机物多组分吸附模式,环境科学学报,1996 年,vol.16,no.2,155-161.
    [65] vol.28,no.1 近海沉积物二组分吸附模式与有机物的吸附,大连理工大学学报,1995,vol.35,no.5,44-48。
    [66] 彭胜,陈家军,王红旗,挥发性有机污染物在土壤中的运移机制与模型,土壤学报,2001 年,vol.38,No.3,315-323。
    [67] 裘祖楠,张仲燕,漆德瑶,苏州河底泥中污染物分布特征及相关性[J],上海环境科学,1998,17(2):10-14。
    [68] Ab-Razak I A, Li A, Christensen E R, et al. Association of PAHs ,PcBs,137Cs with clay, silt and organic carbon in sediments[J]. Water Science & Technology, 1996,34(7-8):29-35.
    [69] 朱利中,徐霞,胡松. 西湖底泥对水中苯胺、苯酚的吸附性能及机理[J].环境科学,2000,20(2):28-31。
    [70] McKenzie S F, Tiller D, allen D. Organochlorine pesticide residues in water and sediments from the Ovens and King rivers, north-east Victoria, Australian[J]. Archives of Environmental Contamination Toxicology, 1994,26(4):483.
    [71] Pignatello J J, Xing B. Mechanisms of slow sorption of organic chemicals to natural particles[J]. Environmental Science and Technology. 1996,30:1-10.
    [72] Farrell J , Reinhard M. Desorption of halogenated organics from model slids, sediments, and soil under unsaturated conditions. 2. Kinetics [J] Environ Sci Techno, 1994,28:63-72.
    [73] Crank J. The mathematics of diffusion;Oxford University Press: Oxford, United Kingdom, 1975.
    [74] Beyer A, Mackay D, et al. Assessing long-Range transport potential of persistent organic pollutants[J]. Environ Sci Technol, 2000, 34:699-703.
    [75] Karapanagioti H K. Impacts of heterogeneous organic matter on phenanthrene sorption: equilibrium and kinetic studies with aquifer material [J]. Environ Sci Technol, 2000, 34:405-414.
    [76] Weber W J, Miller C T. Modeling the sorption of hydrophobic contaminants by aquifer materials. I. Rates and Equilibrium[J]. Water Res, 1988,22,457-464.
    [77] Pedit J A, Miller C T. Heterogeneous sorption processes in subsurface systems. 2.Diffusion modeling approaches[J]. Environ Sci Technol. 1995,29(7):1766.
    [78]周文敏等,水中优先控制污染物黑名单[J]. 中国环境监测,1990,6(4):1-3.
    [79] Weber W J, McGinley P M, Katz L E. sorption phenomena in subsurface systems :concepts, models and effects on contaminants fate and transport[J]. Water res, 1991, 25: 499-528.
    [80] Pedit J A, Miller C T. heterogeneous sorption processes in subsurface systems. 1. Model formulation and applications[J]. Environ Sci Technol,1994,28:2094-2104.
    [81] Schwarzenbach R P, Gschwend P M, Imboden D M, Environmental Organic Chemistry[M]:John wiley & sons: New York, 1993.
    [82] Ball W P, Roberts P v. Sorption rate studies with halogenated organic chemicals and sandy aquifer material. Implications for solute transport and groundwater remediation[C]. National conference on Environmental Engineering, 1990, 307-313.
    [83] Brusseau M L, Rao P S C. sorption kinetics of organic chemicals. Methods, models and mechanisms[J] Soil Science Society of America, 1991,27:281-302.
    [84] Brusseau M L. Effect of nonlinear sorption on transformation of contaminants during transport in porous media[J]. Journal of contaminant Hydrology, 1995,17(4):277.
    [85] Brusseau M L, Rao P S C. sorption of kinetics of organic chemicals. Evaluation of gas-pruge and miscible-displacement techniques [J] Environ Sci Technol, 1990,24(5):727-735.
    [86] Mornier S, Braucher R, Benaim J Y. differentiation of organic matter's properties of the Rio Negro basin by cross-flow ultra-filtration and UV-spectrofluorescence[J]. Water Resarch, 1999,33(10):2363-2373.
    [87] Chiou C T, Lee J F, Boyd S A. Surface are of soil organic matter[J]. Environ Sci Technol, 1990,24:1164-1166.
    [88] Chiou C T, Kile D E, Rutherford D W, Manes M. Sorption of selected organic compounds from water to a peat soil and its humic-acid and humin fractions: potential sources of the sorption nonlinearity[J]. Environ Sci Technol,2000,34(7):1254-1258.
    [89] Xing B, Pignatello J. Time-dependent isotherm shape of organic compounds in soil organic matter: implications for sorption mechanism[J]. Environ Toxicl Chem, 1996,15:1282-1288.
    [90] Xing B, Pignatello J. Dual-mode sorption of low-polarity compounds in glassy poly and soil organic matter[J]. Environ Sci Technol,1997,31:792-799.
    [91] Chen, W, Kan A T, Tomson M B. Irreversible adsorption of chlorinated 苯 s to natural sedimentsL implications for sediment quality criteria[J]. Environ Sci Technol,2000, 34:385-392.
    [92] Paaso N, Peuravuori J, Lehtonen T, Pihlaja K. Sediment-dissolved organic matter equilibrium partitioning of pentachlorophenol: the role of humic acid[J]. environmental International, 2002,28:173-183.
    [93]赵振国,Langmuir 方程在稀溶液吸附中的应用,[J] 大学化学,1999,vol.14,No.5:7-12。
    [94] 杨琛,煤中干酪根的非均质性与疏水性有机污染物的吸附-解吸行为间的关系.[C].中国科学院广州地球化学研究所,2004, 57-63.
    [95] Hrissi.K.Karapanagioti , Impacts of heterogeneous organic matter on phenanthrene sorption: Equilibrium and Kinetic studies with aquifer material.[J]. Environ.Sci.Technol , 2000,34:406-414.
    [96]鲁如坤,土壤农业化学性质分析方法[M],中国农业科技出版社,2004.4。
    [97]王连生等译,环境有机化学[M],化学工业出版社,2004.1:178-215。
    [98]Gustafsson, O., and P.M.Gschwend, The flus of black carbon to surface sediments on the New England continental shelf. [J] Geochim. Cosmochim. Acta, 1998, 62:465-472.

© 2004-2018 中国地质图书馆版权所有 京ICP备05064691号 京公网安备11010802017129号

地址:北京市海淀区学院路29号 邮编:100083

电话:办公室:(+86 10)66554848;文献借阅、咨询服务、科技查新:66554700