Dataset Information

Adsorption of PFOA at the Air-Water Interface during Transport in Unsaturated Porous Media.

ABSTRACT: Miscible-displacement experiments are conducted with perfluorooctanoic acid (PFOA) to determine the contribution of adsorption at the air-water interface to retention during transport in water-unsaturated porous media. Column experiments were conducted with two sands of different diameter at different PFOA input concentrations, water saturations, and pore-water velocities to evaluate the impact of system variables on retardation. The breakthrough curves for unsaturated conditions exhibited greater retardation than those obtained for saturated conditions, demonstrating the significant impact of air-water interfacial adsorption on PFOA retention. Retardation was greater for lower water saturations and smaller grain diameter, consistent with the impact of system conditions on the magnitude of air-water interfacial area in porous media. Retardation was greater for lower input concentrations of PFOA for a given water saturation, consistent with the nonlinear nature of surfactant fluid-fluid interfacial adsorption. Retardation factors predicted using independently determined parameter values compared very well to the measured values. The results showed that adsorption at the air-water interface is a significant source of retention for PFOA, contributing approximately 50-75% of total retention, for the test systems. The significant magnitude of air-water interfacial adsorption measured in this work has ramifications for accurate determination of PFAS migration potential in vadose zones.

SUBMITTER: Lyu Y

PROVIDER: S-EPMC6312111 | biostudies-literature | 2018 Jul

REPOSITORIES: biostudies-literature

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Adsorption of PFOA at the Air-Water Interface during Transport in Unsaturated Porous Media.

Lyu Ying Y Brusseau Mark L ML Chen Wei W Yan Ni N Fu Xiaori X Lin Xueyu X

Environmental science & technology 20180626 14

Miscible-displacement experiments are conducted with perfluorooctanoic acid (PFOA) to determine the contribution of adsorption at the air-water interface to retention during transport in water-unsaturated porous media. Column experiments were conducted with two sands of different diameter at different PFOA input concentrations, water saturations, and pore-water velocities to evaluate the impact of system variables on retardation. The breakthrough curves for unsaturated conditions exhibited great ...[more]

PMID: 29944343

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Project description:The objective of this work was to determine the methods that produce the most representative measurements and estimations of air-water interfacial area specifically for the retention and transport of PFAS and other interfacially active solutes in unsaturated porous media. Published data sets of air-water interfacial areas obtained with multiple measurement and prediction methods were compared for paired sets of porous media comprising similar median grain diameters, but one with solid-surface roughness (sand) and one without roughness (glass beads). All interfacial areas produced with the multiple diverse methods were coincident for the glass beads, providing validation of the aqueous interfacial tracer-test methods. The results of this and other benchmarking analyses demonstrated that the differences in interfacial areas measured for sands and soil by different methods are not due to errors or artifacts in the methods but rather the result of method-dependent differential contributions of solid-surface roughness. The contributions of roughness to interfacial areas measured by interfacial tracer-test methods were quantified and shown to be consistent with prior theoretical and experiment-based investigations of air-water interface configurations on rough solid surfaces. Three new methods for estimating air-water interfacial areas were developed, one based on the scaling of thermodynamic-determined values and the other two comprising empirical correlations incorporating grain diameter or NBET solid surface area. All three were developed based on measured aqueous interfacial tracer-test data. The three new and three existing estimation methods was tested using independent data sets of PFAS retention and transport. The results showed that the method based on treating air-water interfaces as smooth surfaces as well as the standard thermodynamic method produced inaccurate air-water interfacial areas that failed to reproduce the multiple measured PFAS retention and transport data sets. In contrast, the new estimation methods produced interfacial areas that accurately represented air-water interfacial adsorption of PFAS and associated retention and transport. The measurement and estimation of air-water interfacial areas for field-scale applications is discussed in light of these results.

Project description:Per- and poly-fluoroalkyl substances (PFAS) adsorb at air-water interfaces during transport in unsaturated porous media. This can cause surfactant-induced flow and enhanced retention that is a function of concentration, which complicates characterization and modeling of PFAS transport under unsaturated conditions. The influence of surfactant-induced flow and nonlinear air-water interfacial adsorption (AWIA) on PFAS transport was investigated with a series of miscible-displacement transport experiments conducted with a several-log range in input concentrations. Perfluorooctane sulfonic acid (PFOS), perfluorooctanoic acid (PFOA), and ammonium perfluoro 2-methyl-3-oxahexanoate (GenX) were used as model PFAS. The results were interpreted in terms of critical reference concentrations associated with PFAS surface activities and their relationship to the relevancy of transport processes such as surfactant-induced flow and nonlinear AWIA for concentration ranges of interest. Analysis of the measured transport behavior of PFAS under unsaturated-flow conditions demonstrated that AWIA was linear when the input concentration was sufficiently below the critical reference concentration. This includes the absence of significant arrival-front self-sharpening and extended elution tailing of the breakthrough curves, as well as the similarity of retardation factors measured for a wide range of input concentrations. Independently-predicted simulations produced with a comprehensive flow and transport model that accounts for transient variably-saturated flow, surfactant-induced flow, nonlinear rate-limited solid-phase sorption, and nonlinear rate-limited AWIA provided excellent predictions of the measured transport. A series of simulations was conducted with the model to test the specific impact of various processes potentially influencing PFOS transport. The simulation results showed that surfactant-induced flow was negligible and that AWIA was effectively linear when the input concentration was sufficiently below the critical reference concentration. PFAS retention associated with AWIA can be considered to be ideal in such cases, thereby supporting the use of simplified mathematical models. Conversely, apparent nonideal transport behavior was observed for experiments conducted with input concentrations similar to or greater than the critical reference concentration.

Dataset Information

Adsorption of PFOA at the Air-Water Interface during Transport in Unsaturated Porous Media.

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Adsorption of PFOA at the Air-Water Interface during Transport in Unsaturated Porous Media.

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