Citation: | GUO Zhilin, ZHAO Dongwei, PENG Zhanxiang, ZHAI Xuchen. The impact of surface water-groundwater interactions on the fate and transport of typical PFAS[J]. Hydrogeology & Engineering Geology, 2025, 52(3): 1-13. doi: 10.16030/j.cnki.issn.1000-3665.202409027 |
Per- and polyfluoroalkyl substances (PFAS) are a class of ubiquitous and persistent pollutants that pose significant risks to drinking water and human health. Considerable progress has been made in understanding the transport processes of PFAS in soil over the past decade; however, there is a lack of quantitative studies on the migration and transformation of PFAS in groundwater under complex hydrodynamic conditions. This study, focusing on perfluorohexane sulfonate (PFHxS), investigated the migration and transformation mechanisms of PFAS under variably saturated flow conditions. The influence of stratum heterogeneity and water table fluctuations on the migration and transformation of PFHxS in groundwater was explored. By simulating the migration and transformation processes of PFHxS in the aqueous phase, solid phase, and air-water interface, the migration and transformation behavior patterns of PFHxS under surface water-groundwater interaction condition in riparian zone was investigated. The results show that high permeability areas of heterogeneous layers create preferential channels for flow and transport, accelerating the migration of PFHxS to riparian zones The interaction between surface water and groundwater caused by rainfall led to the spatial redistribution of PFHxS pollution plume and extended the coverage of PFHxS pollution area. The presence of preferential flow accelerates the response rate of PFHxS in the surface water-groundwater interaction. This study contributes to enhancing the accuracy of predicting the extent of pollution spread in similar complex environments, optimizing monitoring and response measures, and providing a scientific basis for pollution emergency management.
[1] | BUCK R C,FRANKLIN J,BERGER U,et al. Perfluoroalkyl and polyfluoroalkyl substances in the environment:Terminology,classification,and origins[J]. Integrated Environmental Assessment and Management,2011,7(4):513 − 541. doi: 10.1002/ieam.258 |
[2] | 王佩,黄欣怡,曹致纬,等. 新污染物共排放对生态环境监测和管理的挑战[J]. 环境科学,2022,43(11):4801 − 4809. [WANG Pei,HUANG Xinyi,CAO Zhiwei,et al. Challenges regarding the co-emission of emerging pollutants to eco-environmental monitoring and management[J]. Environmental Science,2022,43(11):4801 − 4809. (in Chinese with English abstract)] WANG Pei, HUANG Xinyi, CAO Zhiwei, et al. Challenges regarding the co-emission of emerging pollutants to eco-environmental monitoring and management[J]. Environmental Science, 2022, 43(11): 4801 − 4809. (in Chinese with English abstract) |
[3] | 金宵卉,阎妮. 全氟及多氟烷基化合物前体物质在环境中迁移与转化行为研究进展[J]. 水文地质工程地质,2024,51(2):35 − 49. [JIN Xiaohui,YAN Ni. Advances in researches on migration and transformation behavior of per-and polyfluoroalkyl substances precursors in the environment[J]. Hydrogeology & Engineering Geology,2024,51(2):35 − 49. (in Chinese with English abstract)] JIN Xiaohui, YAN Ni. Advances in researches on migration and transformation behavior of per-and polyfluoroalkyl substances precursors in the environment[J]. Hydrogeology & Engineering Geology, 2024, 51(2): 35 − 49. (in Chinese with English abstract) |
[4] | BRUSSEAU M L. Assessing the potential contributions of additional retention processes to PFAS retardation in the subsurface[J]. Science of the Total Environment,2018,613/614:176 − 185. doi: 10.1016/j.scitotenv.2017.09.065 |
[5] | LYU Ying,BRUSSEAU M L,CHEN Wei,et al. Adsorption of PFOA at the air–water interface during transport in unsaturated porous media[J]. Environmental Science & Technology,2018,52(14):7745 − 7753. |
[6] | BRUSSEAU M L. Estimating the relative magnitudes of adsorption to solid-water and air/oil-water interfaces for per- and poly-fluoroalkyl substances[J]. Environmental Pollution,2019,254,Part B:113102. |
[7] | COSTANZA J,ARSHADI M,ABRIOLA L M,et al. Accumulation of PFOA and PFOS at the air–water interface[J]. Environmental Science & Technology Letters,2019,6(8):487 − 491. |
[8] | GUO Bo,ZENG Jicai,BRUSSEAU M L. A mathematical model for the release,transport,and retention of per-and polyfluoroalkyl substances (PFAS) in the vadose zone[J]. Water Resources Research,2020,56(2):e2019WR026667. doi: 10.1029/2019WR026667 |
[9] | WANG Zhanyuan,DEWITT J,HIGGINS C P,et al. Correction to “a never-ending story of per- and polyfluoroalkyl substances (PFASs)?”[J]. Environmental Science & Technology,2018,52(5):3325. |
[10] | HUNTER ANDERSON R,ADAMSON D T,STROO H F. Partitioning of poly- and perfluoroalkyl substances from soil to groundwater within aqueous film-forming foam source zones[J]. Journal of Contaminant Hydrology,2019,220:59 − 65. doi: 10.1016/j.jconhyd.2018.11.011 |
[11] | DAUCHY X,BOITEUX V,COLIN A,et al. Deep seepage of per- and polyfluoroalkyl substances through the soil of a firefighter training site and subsequent groundwater contamination[J]. Chemosphere,2019,214:729 − 737. doi: 10.1016/j.chemosphere.2018.10.003 |
[12] | FILIPOVIC M,WOLDEGIORGIS A,NORSTRÖM K,et al. Historical usage of aqueous film forming foam:A case study of the widespread distribution of perfluoroalkyl acids from a military airport to groundwater,lakes,soils and fish[J]. Chemosphere,2015,129:39 − 45. doi: 10.1016/j.chemosphere.2014.09.005 |
[13] | HOISAETER A,PFAFF A,BREEDVELD G D. Leaching and transport of PFAS from aqueous film-forming foam (AFFF) in the unsaturated soil at a firefighting training facility under cold climatic conditions[J]. Journal of Contaminant Hydrology,2019,222:112 − 122. doi: 10.1016/j.jconhyd.2019.02.010 |
[14] | XIAO Feng,SIMCIK M F,HALBACH T R,et al. Perfluorooctane sulfonate (PFOS) and perfluorooctanoate (PFOA) in soils and groundwater of a U S metropolitan area:Migration and implications for human exposure[J]. Water Research,2015,72:64 − 74. doi: 10.1016/j.watres.2014.09.052 |
[15] | WEBER A K,BARBER L B,LEBLANC D R,et al. Geochemical and hydrologic factors controlling subsurface transport of poly- and perfluoroalkyl substances,cape cod,massachusetts[J]. Environmental Science & Technology,2017,51(8):4269 − 4279. |
[16] | 潘明浩,时健,左锐,等. 水位波动下包气带透镜体影响LNAPL迁移的数值模拟研究[J]. 水文地质工程地质,2022,49(1):154 − 163. [PAN Minghao,SHI Jian,ZUO Rui,et al. A numerical simulation study of the effect of the vadose zone with lenses on LNAPL migration under the fluctuating water table[J]. Hydrogeology & Engineering Geology,2022,49(1):154 − 163. (in Chinese with English abstract)] PAN Minghao, SHI Jian, ZUO Rui, et al. A numerical simulation study of the effect of the vadose zone with lenses on LNAPL migration under the fluctuating water table[J]. Hydrogeology & Engineering Geology, 2022, 49(1): 154 − 163. (in Chinese with English abstract) |
[17] | BRUSSEAU M L,YAN Ni,VAN GLUBT S,et al. Comprehensive retention model for PFAS transport in subsurface systems[J]. Water Research,2019,148:41 − 50. doi: 10.1016/j.watres.2018.10.035 |
[18] | GUO Bo,ZENG Jicai,BRUSSEAU M L,et al. A screening model for quantifying PFAS leaching in the vadose zone and mass discharge to groundwater[J]. Advances in Water Resources,2022,160:104102. doi: 10.1016/j.advwatres.2021.104102 |
[19] | BRUSSEAU M L,ANDERSON R H,GUO Bo. PFAS concentrations in soils:Background levels versus contaminated sites[J]. The Science of the Total Environment,2020,740:140017. doi: 10.1016/j.scitotenv.2020.140017 |
[20] | BRUSSEAU M L,VAN GLUBT S. The influence of molecular structure on PFAS adsorption at air-water interfaces in electrolyte solutions[J]. Chemosphere,2021,281:130829. doi: 10.1016/j.chemosphere.2021.130829 |
[21] | LYU Ying,BRUSSEAU M L. The influence of solution chemistry on air-water interfacial adsorption and transport of PFOA in unsaturated porous media[J]. The Science of the Total Environment,2020,713:136744. doi: 10.1016/j.scitotenv.2020.136744 |
[22] | BRUSSEAU M L,VAN GLUBT S. The influence of surfactant and solution composition on PFAS adsorption at fluid-fluid interfaces[J]. Water Research,2019,161:17 − 26. doi: 10.1016/j.watres.2019.05.095 |
[23] | EL OUNI A,GUO Bo,ZHONG Hua,et al. Testing the validity of the miscible-displacement interfacial tracer method for measuring air-water interfacial area:Independent benchmarking and mathematical modeling[J]. Chemosphere,2021,263:128193. doi: 10.1016/j.chemosphere.2020.128193 |
[24] | ZENG Jicai,BRUSSEAU M L,GUO Bo. Model validation and analyses of parameter sensitivity and uncertainty for modeling long-term retention and leaching of PFAS in the vadose zone[J]. Journal of Hydrology,2021,603:127172. doi: 10.1016/j.jhydrol.2021.127172 |
[25] | ZENG J,GUO Bo. Reduced accessible air–water interfacial area accelerates PFAS leaching in heterogeneous vadose zones[J]. Geophysical Research Letters,2023,50(8):e2022GL102655. doi: 10.1029/2022GL102655 |
[26] | HITZELBERGER M,KHAN N A,MOHAMED R A M,et al. PFOS mass flux reduction/mass removal:Impacts of a Lower-permeability sand lens within otherwise homogeneous systems[J]. Environmental Science & Technology,2022,56(19):13675 − 13685. |
[27] | ZENG Jicai,GUO Bo. Multidimensional simulation of PFAS transport and leaching in the vadose zone:Impact of surfactant-induced flow and subsurface heterogeneities[J]. Advances in Water Resources,2021,155:104015. doi: 10.1016/j.advwatres.2021.104015 |
[28] | 吴佩鹏,束龙仓,李福林,等. 层状非均质性影响下河流对地下水的补给过程研究[J]. 水文地质工程地质,2023,50(3):44 − 53. [WU Peipeng,SHU Longcang,LI Fulin,et al. Influence of stratified heterogeneity on the recharge from surface water to groundwater[J]. Hydrogeology & Engineering Geology,2023,50(3):44 − 53. (in Chinese with English abstract)] WU Peipeng, SHU Longcang, LI Fulin, et al. Influence of stratified heterogeneity on the recharge from surface water to groundwater[J]. Hydrogeology & Engineering Geology, 2023, 50(3): 44 − 53. (in Chinese with English abstract) |
Two-dimensional geological profile of the riparian zone and boundary and initial conditions
Heterogeneous alluvium in two different riparian zones and 9 observation points near the riverbank
Rainfall and changes in groundwater level at the left boundary and river water level
Flow field distribution during PFAS release
Distribution of PFHxS at aqueous phase, solid phase adsorption, and air-water interface at 3, 6, and 10 years of continuous release of PFHxS (hom, het1 and het2 in alluvial layer)
Profile flow field during rainfall
PFHxS concentration in the subsurface environment during the surface water-groundwater interaction compared with the PFHxS concentration distribution at the initial moment
Under different formation conditions, the concentration change curves of total PFHxS concentration per unit volume, aqueous phase concentration, solid phase adsorption concentration, and air-water interface adsorption concentration during the surface water-groundwater interaction
Concentration varies of PFHxS at x=42 m section under different formation conditions
Velocity distribution near the riparian zone in different strata on 99 d
Under different stratigraphic conditions, the distributions of PFHxS near the riparian zone following surface water recharge to groundwater (60 days) and after a prolonged heavy rainfall event (115 days)