空气-水界面塌陷和速率受限的固体解吸控制了从地下渗流带沥滤全氟烷基酸的过程

IF 3.5 3区 环境科学与生态学 Q2 ENVIRONMENTAL SCIENCES
John F. Stults , Charles E. Schaefer , Yida Fang , Julie Devon , Dung Nguyen , Isreq Real , Shilai Hao , Jennifer L. Guelfo
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引用次数: 0

摘要

一些全氟烷基和多氟烷基物质 (PFAS) 由于同时吸附在土壤和空气-水界面上,因此会被强烈保留在地下水层中。虽然已有大量研究致力于了解这些多相保留过程的平衡行为,但在实地相关条件下,受水成膜泡沫(AFFF)影响的土壤中的浸出和解吸行为可能会明显偏离平衡状态。在此,我们利用实地收集的受 AFFF 影响的土壤进行了实验室柱研究,以考察在模拟降雨条件下全氟烷基酸 (PFAAs) 的沥滤情况。对 HYDRUS 1-D 模型进行了校准,以使用多种边界条件估算分层系统中土壤的非饱和水力特性。利用 HYDRUS 模型和简化的质量平衡计算对 PFAS 的平衡分配进行了前向模拟,结果显示与 PFAS 柱外净质量通量非常吻合。但是,这两种方法都无法预测浸出孔隙水中的 PFAS 浓度。为了更好地了解控制浸出行为的机制,我们采用了 HYDRUS 1-D 两点浸出模型,其中包含固相速率限制和平衡空气-水界面分配。通过内置的数值反演,考虑了包含不同形式的气水界面平衡分区的新型模型的三种变体。数值反演结果表明,结合空气-水界面塌陷和土壤中的速率限制解吸,可以更好地预测全氟辛烷磺酸在受 AFFF 影响的土壤中表现出的独特浸出行为。对初始条件和限速解吸项进行了敏感性分析,以评估模型与测量数据的一致性。本文所展示的模型表明,在某些情况下,实验室平衡分配数据可以对总沥滤量进行合理估算,但却无法解释影响非饱和土壤中 PFAA 向地下水沥滤的重要速率限制和非 Fickian 迁移。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Air-water interfacial collapse and rate-limited solid desorption control Perfluoroalkyl acid leaching from the vadose zone

Some Per- and polyfluoroalkyl substances (PFAS) are strongly retained in the vadose zone due to their sorption to both soils and air-water interfaces. While significant research has been dedicated to understanding equilibrium behavior for these multi-phase retention processes, leaching and desorption from aqueous film-forming foam (AFFF) impacted soils under field relevant conditions can exhibit significant deviations from equilibrium. Herein, laboratory column studies using field collected AFFF-impacted soils were employed to examine the leaching of perfluoroalkyl acids (PFAAs) under simulated rainfall conditions. The HYDRUS 1-D model was calibrated to estimate the unsaturated hydraulic properties of the soil in a layered system using multiple boundary condtions. Forward simulations of equilibrium PFAS partitioning using the HYDRUS model and simplified mass balance calculations showed good agreement with the net PFAS mass flux out of the column. However, neither were able to predict the PFAS concentrations in the leached porewater. To better understand the mechanisms controlling the leaching behavior, the HYDRUS 1-D two-site leaching model incorporating solid phase rate limitation and equilibrium air-water interfacial partitioning was employed. Three variations of the novel model incorporating different forms of equilibrium air-water interfacial partitioning were considered using built-in numerical inversion. Results of numerical inversion show that a combination of air-water interfacial collapse and rate-limited desorption from soils can better predict the unique leaching behavior exhibited by PFAAs in AFFF-impacted soils. A sensitivity analysis of the initial conditions and rate-limited desorption terms was conducted to assess the agreement of the model with measured data. The models demonstrated herein show that, under some circumstances, laboratory equilibrium partitioning data can provide a reasonable estimation of total mass leaching, but fail to account for the significant rate-limited, non-Fickian transport which affect PFAA leaching to groundwater in unsaturated soils.

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来源期刊
Journal of contaminant hydrology
Journal of contaminant hydrology 环境科学-地球科学综合
CiteScore
6.80
自引率
2.80%
发文量
129
审稿时长
68 days
期刊介绍: The Journal of Contaminant Hydrology is an international journal publishing scientific articles pertaining to the contamination of subsurface water resources. Emphasis is placed on investigations of the physical, chemical, and biological processes influencing the behavior and fate of organic and inorganic contaminants in the unsaturated (vadose) and saturated (groundwater) zones, as well as at groundwater-surface water interfaces. The ecological impacts of contaminants transported both from and to aquifers are of interest. Articles on contamination of surface water only, without a link to groundwater, are out of the scope. Broad latitude is allowed in identifying contaminants of interest, and include legacy and emerging pollutants, nutrients, nanoparticles, pathogenic microorganisms (e.g., bacteria, viruses, protozoa), microplastics, and various constituents associated with energy production (e.g., methane, carbon dioxide, hydrogen sulfide). The journal''s scope embraces a wide range of topics including: experimental investigations of contaminant sorption, diffusion, transformation, volatilization and transport in the surface and subsurface; characterization of soil and aquifer properties only as they influence contaminant behavior; development and testing of mathematical models of contaminant behaviour; innovative techniques for restoration of contaminated sites; development of new tools or techniques for monitoring the extent of soil and groundwater contamination; transformation of contaminants in the hyporheic zone; effects of contaminants traversing the hyporheic zone on surface water and groundwater ecosystems; subsurface carbon sequestration and/or turnover; and migration of fluids associated with energy production into groundwater.
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