Model validation and analyses of parameter sensitivity and uncertainty for modeling long-term retention and leaching of PFAS in the vadose zone

Zeng, Jicai; Brusseau, Mark L.; Guo, Bo

doi:10.1016/j.jhydrol.2021.127172

Cited by 62Per- and polyfluoroalkyl substances researchGroundwater flow and contamination studiesSoil and Unsaturated Flow

Model validation and analyses of parameter sensitivity and uncertainty for modeling long-term retention and leaching of PFAS in the vadose zone

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Zeng, Jicai, Brusseau, Mark L., Guo, Bo·2021·Journal of Hydrology

DOI 10.1016/j.jhydrol.2021.127172

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Abstract

PFAS are emerging contaminants widespread in the environment. As surfactants, PFAS tend to accumulate at solid–water and air–water interfaces in the vadose zone, which may pose long-term threats to groundwater. The primary factors that control the long-term retention of PFAS in the vadose zone remain poorly understood. To address this knowledge gap, we first use multiple datasets from transport experiments to validate a state-of-theart mathematical model that incorporates transient variably saturated flow, surfactant-induced flow, and ratelimited and nonlinear solid-phase and air–water interfacial adsorption. We then employ the validated model to simulate and analyze the primary processes and parameters controlling the retention and leaching of PFAS in the vadose zone at a model fire-training-area site. Our simulations show that adsorption at solid–water and air–water interfaces leads to strong retention of PFAS in the vadose zone. The strength of retention increases with PFAS chain length and porewater ionic strength, while it decreases at greater PFAS concentrations due to nonlinear adsorption. Comprehensive parameter sensitivity analyses reveal that model predictions are most sensitive to parameters related to the air–water interfacial area and PFAS interfacial properties when air–water interfacial adsorption (AWIA) is more important than solid-phase adsorption (SPA). Predicted PFAS leaching rates vary by a wide range resulting from uncertainties in the input parameters, but the uncertainty range is much greater for longer-chain PFAS than that of their shorter-chain counterparts. The simulated arrival times to groundwater were found to follow log-normal distributions. Finally, model complexity analysis reveals that nonlinearity in AWIA and kinetic SPA and kinetic AWIA have a minimal impact on the long-term retention of PFAS under the wide range of field conditions examined in the present study.

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Inhomogeneities significantly influenced PFAS transport behaviour in synthetic soil profiles; preferential flow enhanced saturation along pathways, reduced air-water interfacial area and PFAS sorption, and greatly enhanced PFAS travel times.
“Zeng and Guo (2021) were able to demonstrate on the basis of synthetic soil profiles that inhomogeneities significantly influenced the PFAS transport behaviour within the considered profiles.Preferential flow enhanced the saturation along pathways which consequently reduced the air water interfacial area and therefore PFAS sorption, leading to greatly enhance PFAS travel times.”
From Model-based identification of vadose zone controls on PFAS mobility under semi-arid climate conditions (2022) · cites this paper as Zeng and Guo (2021)
Elevated PFAS concentration may reduce surface tension leading to enhanced surfactant induced flow (SIF).
“while elevated PFAS concentration itself may reduce surface tension leading to enhanced surfactant induced flow (SIF) (e.g.Costanza-Robinson and Henry, 2017; Zeng and Guo, 2021).”
From Model-based identification of vadose zone controls on PFAS mobility under semi-arid climate conditions (2022) · cites this paper as Zeng and Guo, 2021
The modified LEACHM code does not take surfactant-induced flow (SIF) into account; this simplification was based on results showing minimal SIF effects at PFAS concentrations up to ~10 mg/L.
“In addition, the modified LEACHM code does not take surfactant-induced flow (SIF) into account.This simplification was based on results by Zeng and Guo (2021) who demonstrated that acceleration of vertical leaching and lateral spreading of PFAS resulting from SIF was minimal even under strongly elevated PFAS porewater concentrations of up to ~ 10 mg/L.Silva et al. (2020) derived at similar finding”
From Model-based identification of vadose zone controls on PFAS mobility under semi-arid climate conditions (2022) · cites this paper as Zeng and Guo (2021)
The maximum surface areas calculated by the modified geometric mean particle diameter approach are in general agreement with literature and compared well against Ethylene-Glycol and BET isotherm methods evaluated on 21 different soils.
“This provided maximum surface areas which are in general agreement with those reported in the relevant literature (Fig. 6 and e.g.Silva et al. 2020;Zeng and Guo, 2021) and which compared well against two frequently used surface area quantification methods, i.e. the Ethylene-Glycol and BET isotherm method evaluated on the basis of 21 different soils (Supporting Information A).”
From Model-based identification of vadose zone controls on PFAS mobility under semi-arid climate conditions (2022) · cites this paper as Zeng and Guo, 2021
The AWI sorption capability of the extended LEACHM code has been successfully benchmarked against Guo et al. (2020) and Zeng et al. (2021).
“The AWI sorption capability of the extended LEACHM code has been successfully benchmarked against Guo et al. (2020) and Zeng et al. (2021”
From Model-based identification of vadose zone controls on PFAS mobility under semi-arid climate conditions (2022) · cites this paper as Zeng et al. (2021)

Theoretical simulations have identified variability in the air-water interface and associated partitioning of PFAS as the strongest controls on PFAS transport in the subsurface, but time series data to confirm this at field sites are lacking.
“Theoretical simulations have identified variability in the air–water interface and associated partitioning of PFAS as the strongest controls on PFAS transport in the subsurface, but time series data to confirm this at field sites are lacking.33,34”
From Centurial Persistence of Forever Chemicals at Military Fire Training Sites (2023) · cites this paper as [33]
These results agree with mathematical and experimental evidence showing much larger solids retention of PFAS under unsaturated compared to saturated conditions.
“These results agree with mathematical and experimental evidence showing much larger solids retention of PFAS under unsaturated compared to saturated conditions.14,33”
From Centurial Persistence of Forever Chemicals at Military Fire Training Sites (2023) · cites this paper as [33]
Concentration dependency of these coefficients has been observed in prior experimental work but has been shown to have minimal impact on long-term environmental behavior.
“Concentration dependency of these coefficients has been observed in prior experimental work but has been shown to have minimal impact on long-term environmental behavior.33”
From Centurial Persistence of Forever Chemicals at Military Fire Training Sites (2023) · cites this paper as [33]
These dynamic changes of porewater concentration due to transient water infiltration are consistent with those reported in prior work.
“These dynamic changes of porewater concentration due to transient water infiltration are consistent with those reported in our prior work (Guo et al., 2020; Zeng et al., 2021).”
From PFAS concentrations in soil versus soil porewater: Mass distributions and the impact of adsorption at air-water interfaces (2022) · cites this paper as Zeng et al., 2021

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Solution Properties of Sodium Perfluoroalkanoates. Heats of Solution, Viscosity B Coefficients, and Surface Tensions
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Per‐ and Polyfluoroalkyl Substances (PFAS) in Subsurface Environments: Occurrence, Fate, Transport, and Research Prospect
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Centurial Persistence of Forever Chemicals at Military Fire Training Sites
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Dynamic Storage, Release, and Enrichment of some Per‐ and Polyfluoroalkyl Substances in the Groundwater Table Fluctuation Zone: Transport Processes Requiring Further Consideration
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PFOS Mass Flux Reduction / Mass Removal: Impacts of Lower Permeability Sand Lens Within Otherwise Homogeneous Systems
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Influence of Tension-Driven Flow on the Transport of AFFF in Unsaturated Media
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Combining field datasets and mathematical modeling to quantify PFAS leaching and mass discharge at an AFFF-impacted site
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Modeling and Evaluation of PFOS Retention in the Unsaturated Zone above the Water Table
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Electrostatic and Chemical Interplay between Air–Water and Mineral–Water Interfaces during PFOS Transport in Unsaturated Porous Media
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Consideration of Vadose Zone Moisture Dynamics in Remediation of PFAS‐Impacted Soils
Askarani, K. K., Cook, J. S., Connor, J. A., & Newell, C. J. (2024) · Groundwater Monitoring & Remediation · doi:10.1111/gwmr.12646 · Cited by 9 · see citing works
Semi-analytical solutions for nonequilibrium transport and transformation of PFAS and other solutes in heterogeneous vadose zones with structured porous media
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Challenges and opportunities for porous media research to address PFAS groundwater contamination
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Mobility of Fluoride and Fluorocarbons in the Soil
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Bridging Science and Practice: Literature Review and Expert Insights on Per‐ and Polyfluoroalkyl Substances Transport Modeling
Gharehveran, M. M., Torres, F., Stults, J. F., Adamson, D. T., Divine, C. E., Naylor, E., Xia, Z., & Anderson, R. H. (2025) · Remediation Journal · doi:10.1002/rem.70042 · Cited by 5 · see citing works
Effects of transient air-water interfacial area on PFOA transport in unsaturated soil
Klevan, C., Garza‐Rubalcava, U., Abriola, L. M., & Pennell, K. D. (2026) · Journal of Contaminant Hydrology · doi:10.1016/j.jconhyd.2026.104859 · Cited by 5 · see citing works
Second-order accurate implicit finite volume method for two-dimensional modeling of PFAS transport in unsaturated porous media with variable surface tension
Wu, R. Z., Li, X., Sun, Y., Szymczak, P., & Jiao, W. (2023) · Advances in Water Resources · doi:10.1016/j.advwatres.2023.104490 · Cited by 5 · see citing works
Multi-compound PFAS transport in the unsaturated zone during infiltration cycles
Kolade, S. O., Ronen, A., Turkeltaub, T., Tsakiroglou, C. D., Klint, K. E., Das, P., & Dahan, O. (2025) · Water Research · doi:10.1016/j.watres.2025.124463 · Cited by 4 · see citing works
Per- and polyfluoroalkyl substances (PFAS) transport from biosolids-amended soils: An experimental and numerical approach
Doria-Manzur, A., Gray, E. P., Streets, S. S., & Guelfo, J. L. (2025) · Water Research · doi:10.1016/j.watres.2025.124674 · Cited by 4 · see citing works
Modeling per- and polyfluoroalkyl substance precursor transformation in groundwater at a well-characterized site
Stockwell, E. B., Adamson, D. T., Gamlin, J. D., Kulkarni, P. R., Singh, A., Falta, R. W., & Newell, C. J. (2025) · Journal of Contaminant Hydrology · doi:10.1016/j.jconhyd.2025.104766 · Cited by 6 · see citing works
Sensitivity of mass flux reduction and mass removal of perfluoroalkyl substances to groundwater flow and transport parameter variability and heterogeneity
Mohamed, R. A. M., Soltanian, M. R., Wang, D., & Carroll, K. C. (2024) · Journal of Hydrology · doi:10.1016/j.jhydrol.2024.132268 · Cited by 4 · see citing works
National collaborative study on the incidence and mobility of PFAS following land application of biosolids
Pepper, I. L., Prasek, S. M., Chorover, J., Prevatt, F. J., Barrientes, D. M., Kester, G., & Brusseau, M. L. (2025) · The Science of The Total Environment · doi:10.1016/j.scitotenv.2025.181197 · Cited by 3 · see citing works
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Application Of Machine Learning To Understand Pfas Occurrence, Distribution, Transport And Removal In WaterPreprint
Ajao, A. (2024) · Preprints.org · doi:10.20944/preprints202403.0627.v1 · Cited by 2 · see citing works
Numerical Experiments for Surfactant Infiltration in the Vadose Zone to Demonstrate Concentration-Dependent Capillarity, Viscosity, and Sorption Characteristics
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Fate and transport of perfluorooctane sulfonic acid (PFOS) within heterogenous riparian floodplains
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Concepts and methods for developing site-specific soil screening levels for per and polyfluoroalkyl substances
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Impacts of Climate Change on Groundwater Quality in the Northern Atlantic Coastal Plain: A Review
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Modelling Per- and Polyfluoroalkyl Substance Precursor Transformation in Groundwater at a Well-Characterized SitePreprint
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A framework for determining site-specific soil screening levels for PFAS
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Reconstructing chlorinated solvent release histories in the vadose zone for groundwater pollution assessment using tree-ring dendrochemistry
Hu, T., Ma, Y., Wang, Y., Liu, S., Ren, J., Jia, X., Wang, H., xu, C., & Hou, D. (2026) · Journal of Hydrology · doi:10.1016/j.jhydrol.2026.135166
Data assimilation for PFOA transport in vadose zone using EnKF with modified HYDRUS-1D
Wang, S., & Tong, J. (2026) · Stochastic environmental research and risk assessment (Print) · doi:10.1007/s00477-026-03262-7
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Sedghi, M. M., & Zhan, H. (2026) · Journal of Contaminant Hydrology · doi:10.1016/j.jconhyd.2026.105031
Evaluating the saturated paste extraction method for determining PFAS solid-liquid partitioning coefficients (Kd) in low-organic-carbon sand aquifers.
Liljeström, O., Berggren-Kleja, D., Ellbrant, M., Pettersson, M., Enell, A., & Ahrens, L. (2026) · Environmental Pollution · doi:10.1016/j.envpol.2026.128851
When does the vadose zone control watershed PFAS delivery to groundwater? Explicit unsaturated-zone transport across shallow, intermediate, and deep AFFF end-membersPreprint
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Multidimensional simulation of PFAS transport and leaching in the vadose zone: impact of surfactant-induced flow and soil heterogeneitiesPreprint
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Authors: Zeng, J., Brusseau, M. L., & Guo, B.
Affiliations: University of Arizona (US)
Corresponding author: Guo, Bo
ORCID: Zeng, Jicai
Brusseau, Mark L.
Guo, Bo
Venue: Journal of Hydrology
Publisher: Elsevier BV
Published: 2021-12
Volume: 603
Pages: 127172
ISSN: 0022-1694 (ISSN-L)
DOI: 10.1016/j.jhydrol.2021.127172
OpenAlex: W3212458978
Semantic Scholar: 336aa1d6fbad146c3491c2f3a52f4280977aa638
Cited by: 62
References: 103
Citations by year: 2026: 11 · 2025: 13 · 2024: 19 · 2023: 11 · 2022: 8
FWCI: 3.58
Type: journal article
Language: en
Open access: bronze
doi.org
Licence: www.elsevier.com/tdm/userlicense/1.0/ (tdm)
www.elsevier.com/legal/tdmrep-license (tdm)
www.elsevier.com/open-access/userlicense/1.0/ (am, 370 d)
doi.org/10.15223/policy-017 (stm-asf)
doi.org/10.15223/policy-037 (stm-asf)
doi.org/10.15223/policy-012 (stm-asf)
doi.org/10.15223/policy-029 (stm-asf)
doi.org/10.15223/policy-004 (stm-asf)
Locations: Journal of Hydrology (acceptedVersion)
UA Campus Repository (The University of Arizona) (acceptedVersion)
Funders: Environmental Security Technology Certification Program (ER21-5041)
National Science Foundation (2023351)
National Institute of Environmental Health Sciences (P42 ES 4940)
Topics: Physical Sciences › Environmental Science › Environmental Chemistry › Per- and polyfluoroalkyl substances research
Physical Sciences › Environmental Science › Environmental Engineering › Groundwater flow and contamination studies
Physical Sciences › Engineering › Civil and Structural Engineering › Soil and Unsaturated Flow
Keywords: PFAS, per- and polyfluoroalkyl substances, vadose zone, long-term retention, leaching, air-water interface adsorption, solid-phase adsorption, variably saturated flow, nonlinear sorption, parameter sensitivity, uncertainty analysis, groundwater contamination, ionic strength, arrival time distribution

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Model validation and analyses of parameter sensitivity and uncertainty for modeling long-term retention and leaching of PFAS in the vadose zone

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