全氟磺酸类物质在沙质沉积物中的迁移规律
Transport behavior of perfluorinated sulfonic acids in sandy sediment
-
摘要: 本工作的目的在于研究全氟磺酸类物质(PFSAs)在典型地下沙质含水层沉积物中的迁移规律,以便于更好地了解地下水中PFSAs的来源和控制措施.通过柱迁移实验获得全氟己烷磺酸(PFHxS)、全氟庚烷磺酸(PFHpS)、全氟辛烷磺酸(n-PFOS)及其两种同分异构体(iso-PFOS-1和iso-PFOS-2)的穿透曲线;用HYDRUS-1D软件中不同的数学模型来模拟穿透曲线,对比确定了最优模拟模型,通过反演推算获取运移参数;并对比了不同PFSAs的迁移规律.研究结果表明,线性一级两位非平衡吸附模型是最优的模拟模型;不同PFSAs的迁移速率有较大的区别:当水流动1000 m时,PFHxS,PFHpS,n-PFOS,iso-PFOS-1和iso-PFOS-2分别迁移了457.1、84.4、67.1、250.8、280.1 m;这种差异与PFSAs分子结构引起的表面吸附特性与分子扩散速率相关.Abstract: This study aimed to investigate the transport behavior of perfluorinated sulfonic acids (PFSAs) in typical sandy provide sediment, and provide better understanding about the source and control of PFSAs pollution in groundwater. Miscible displacement experiments were conducted, and the breakthrough curves of perfluorohexane sulfonate (PFHxS), perfluoroheptane sulfonate (PFHpS), perfluorooctane sulfonate (PFOS) and its two isomers (iso-PFOS-1 and iso-PFOS-2), were simulated using different models coupled in HYDRUS-1D software. The best simulation model was determined and the transport parameters were computed by inverse estimation. Results showed that the linear first-order two-site non-equilibrium adsorption model was most suitable for the simulation of PFSAs transport in sandy aquifer sediment. And the transport velocities of PFSAs were remarkably different. When water flowed 1000 m, PFHxS, PFHpS, PFOS, iso-PFOS-1, and iso-PFOS-2 moved 457.1, 84.4, 67.1, 250.8, and 280.1 m, respectively. These differences were related to the surface sorption characteristics and molecular diffusion rate of PFSAs due to their different molecular structures.
-
Key words:
- perfluorinated sulfonic acids /
- sorption /
- transport /
- sediment /
- HYDRUS-1D /
- breakthrough curve
-
-
[1] 王懿. 持久性全氟化合物典型污染源环境污染特性研究[D].南京:南京农业大学学位论文,2011. WANG Y. Research on persistent perfluorinated compounds environmental contamination characteristics in typical pollution sources[D]. Nanjing: Nanjing Agricultural University,2011(in Chinese). [2] 赵丽霞. 典型全氟化合物在沉积物中的分配行为与微观机制研究[D].天津:南开大学学位论文,2013. ZHAO L X.The study about partition behaviors and mechanisms of typical perfluoroalkyl substances in sedement[D].Tianjin: Nankai University,2013(in Chinese). [3] 祝玉杰,陈来国,高博,等. 大气中全氟与多氟有机化合物研究进展[J]. 环境化学,2015,34(8): 1396-1407. ZHU Y J,CHEN L G,GAO B,et al.Research advance on per- and poly-fluorinated organic compounds in the atmosphere[J].Environmental Chemistry,2015,34(8): 1396-1407(in Chinese).
[4] LU G H,YANG Y L,TANIYASU S,et al. Potential exposure of perfluorinated compounds to Chinese in Shenyang and Yangtze River Delta areas[J]. Environmental Chemistry,2011,8(4): 407-418. [5] MEYER T,DE SILVA A O,SPENCER C,et al. Fate of perfluorinated carboxylates and sulfonates during snowmelt within an Urban Watershed[J]. Environmental Science & Technology,2011,45(19): 8113-8119. [6] SCHULTZ M M,BAROFSKY D F,FIELD J A. Quantitative determination of fluorotelomer sulfonates in groundwater by LC MS/MS[J]. Environmental Science & Technology,2004,38(6): 1828-1835. [7] KURODA K,MURAKAMI M,OGUMA K,et al. Investigating sources and pathways of perfluoroalkyl acids (PFAAs) in aquifers in Tokyo using multiple tracers[J]. Science of the Total Environment,2014,488: 51-60. [8] LONG E R,DUTCH M,WENKLAND S,et al. Quantification of pharmaceuticals,personal care products,and perfluoroalkyl substances in the marine sediments of Puget Sound,Washington,USA[J]. Environmental Toxicology and Chemistry,2013,32(8): 1701-1710. [9] WANG S L,WANG H,DENG W J. Perfluorooctane sulfonate (PFOS) distribution and effect factors in the water and sediment of the Yellow River Estuary,China[J]. Environmental Monitoring and Assessment,2013,185(10): 8517-8524. [10] AWAD E,ZhANG X M,BHAVSAR S P,et al. Long-term environmental fate of perfluorinated compounds after accidental release at toronto airport[J]. Environmental Science & Technology,2011,45(19): 8081-8089. [11] 高珂,傅建捷,高燕,等. 武汉市某高校学生血清中全氟烷酸水平及暴露途径初步研究[J]. 环境化学,2015,34(8): 1424-1432. GAO K,BO J J,GAO Y,et al.A preliminary study on perfluoroalkyl acids levels in serum and exposure pathways for students from a university in Wuhan[J].Environmental Chemistry,2015,34(8): 1424-1432(in Chinese).
[12] MURAKAMI M,KURODA K,SATO N,et al.Groundwater Pollution by Perfluorinated Surfactants in Tokyo[J]. Environmental Science & Technology,2009,43(10): 3480-3486. [13] LINDSTROM A B,STRYNAR M J,DELINSKY A D,et al.Application of WWTP biosolids and resulting perfluorinated compound contamination of surface and well water in Decatur,Alabama,USA[J]. Environmental Science & Technology,2011,45(19): 8015-8021. [14] 邰托娅,王金生,王业耀. 全氟化合物在沉积物中的分布特征及吸附行为[J]. 环境科学与技术,2013,36(11): 96-102. TAI T Y,WANG J S,WANG Y Y.Distribution and sorption of perfluorinated compounds in sediment[J].Environmental Science & Technology,2013,36(11): 96-102(in Chinese).
[15] POOTHOONG S,BOONTANON S K,BOONTANON N. Extraction procedure optimization for perfluorooctane sulfonate and perfluorooctanoic acid in food packaging determination by LC-MS/MS[J]. Journal of Environmental Science and Health Part B-Pesticides Food Contaminants and Agricultural Wastes,2013,48(10): 830-835. [16] SAITO K,UEMURA E,ISHIZAKAI A,et al. Determination of perfluorooctanoic acid and perfluorooctane sulfonate by automated in-tube solid-phase microextraction coupled with liquid chromatography-mass spectrometry[J]. Analytica Chimica Acta,2010,658(2): 141-146. [17] HIGGINS C P,LUTHY R G. Sorption of perfluorinated surfactants on sediments[J]. Environmental Science & Technology,2006,40(23): 7251-7256. [18] CHENG H,ZHANG C,YU Y X,et al. Sorption of perfluorooctane sulfonate (PFOS) on marine sediments[J]. Marine Pollution Bulletin,2012,64(5): 902-906. [19] BURKE V,TREUMANN S,DUENNBIER U,et al. Sorption behavior of 20 wastewater originated micropollutants in groundwater-Column experiments with pharmaceutical residues and industrial agents[J]. Journal of Contaminant Hydrology,2013,154: 29-41. [20] LANGLOIS I,OEHME M. Structural identification of isomers present in technical perfluorooctane sulfonate by tandem mass spectrometry[J]. Rapid Communications in Mass Spectrometry,2006,20(5): 844-850. [21] MARAQA M A,ZHAO X D,LEE J U,et al. Comparison of nonideal sorption formulations in modeling the transport of phthalate esters through packed soil columns[J]. Journal of Contaminant Hydrology,2011,125(1-4): 57-69. [22] SHACKELFORD C D. Laboratory diffusion testing for waste disposal-A review[J]. Journal of Contaminant Hydrology,1991,7(3): 177-217. [23] LABADIE P,CHEVREUIL M. Partitioning behaviour of perfluorinated alkyl contaminants between water,sediment and fish in the Urge River (nearby Paris,France)[J]. Environmental Pollution,2011,159(2): 391-397. [24] LIU H,ZHANG D,LI M J,et al. Competitive adsorption and transport of phthalate esters in the clay layer of JiangHan plain,China[J]. Chemosphere,2013,92(11): 1542-1549. -

计量
- 文章访问数: 1249
- HTML全文浏览数: 1101
- PDF下载数: 540
- 施引文献: 0