Investigating rate-limited sorption, sorption to air–water interfaces, and colloid-facilitated transport during PFAS leaching
Various sorption processes affect leaching of per- and polyfluoroalkyl substances (PFAS) such as PFOA and PFOS. The objectives of this study are to (1) compare rate-limited leaching in column and lysimeter experiments, (2) investigate the relevance of sorption to air–water interfaces (AWI), and (3)...
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description | Various sorption processes affect leaching of per- and polyfluoroalkyl substances (PFAS) such as PFOA and PFOS. The objectives of this study are to (1) compare rate-limited leaching in column and lysimeter experiments, (2) investigate the relevance of sorption to air–water interfaces (AWI), and (3) examine colloid-facilitated transport as a process explaining early experimental breakthrough. A continuum model (CM) with two-domain sorption is used to simulate equilibrium and rate-limited sorption. A random walk particle tracking (PT) model was developed and applied to analyze complex leaching characteristics. Results show that sorption parameters derived from column experiments underestimate long-term PFOA leaching in lysimeter experiments due to early depletion, suggesting that transformation of precursors contributes to the observed long-term leaching in the lysimeters (approximately 0.003 µg/kg/d PFOA). Both models demonstrate that sorption to AWI is the dominant retention mechanism for PFOS in lysimeter experiments, with retardation due to AWI being 3 (CM) to 3.7 (PT) times higher than retardation due to solid phase sorption. Notably, despite a simplified conception of AWI sorption, the PT results are closer to the observations. The PT simulations demonstrate possible colloid-facilitated transport at early time; however, results using substance-specific varying transport parameters align better with the observations, which should be equal if colloid-facilitated transport without additional kinetics is the sole mechanism affecting early breakthrough. Possibly, rate-limited sorption to AWI is relevant during the early stages of the lysimeter experiment. Our findings demonstrate that rate-limited sorption is less relevant for long-term leaching under field conditions compared to transformation of precursors and that sorption to AWI can be the dominant retention mechanism on contaminated sites. Moreover, they highlight the potential of random walk particle tracking as a practical alternative to continuum models for estimating the relative contributions of various retention mechanisms. |
doi_str_mv | 10.1007/s11356-023-30811-2 |
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The objectives of this study are to (1) compare rate-limited leaching in column and lysimeter experiments, (2) investigate the relevance of sorption to air–water interfaces (AWI), and (3) examine colloid-facilitated transport as a process explaining early experimental breakthrough. A continuum model (CM) with two-domain sorption is used to simulate equilibrium and rate-limited sorption. A random walk particle tracking (PT) model was developed and applied to analyze complex leaching characteristics. Results show that sorption parameters derived from column experiments underestimate long-term PFOA leaching in lysimeter experiments due to early depletion, suggesting that transformation of precursors contributes to the observed long-term leaching in the lysimeters (approximately 0.003 µg/kg/d PFOA). Both models demonstrate that sorption to AWI is the dominant retention mechanism for PFOS in lysimeter experiments, with retardation due to AWI being 3 (CM) to 3.7 (PT) times higher than retardation due to solid phase sorption. Notably, despite a simplified conception of AWI sorption, the PT results are closer to the observations. The PT simulations demonstrate possible colloid-facilitated transport at early time; however, results using substance-specific varying transport parameters align better with the observations, which should be equal if colloid-facilitated transport without additional kinetics is the sole mechanism affecting early breakthrough. Possibly, rate-limited sorption to AWI is relevant during the early stages of the lysimeter experiment. Our findings demonstrate that rate-limited sorption is less relevant for long-term leaching under field conditions compared to transformation of precursors and that sorption to AWI can be the dominant retention mechanism on contaminated sites. Moreover, they highlight the potential of random walk particle tracking as a practical alternative to continuum models for estimating the relative contributions of various retention mechanisms.</description><identifier>ISSN: 1614-7499</identifier><identifier>ISSN: 0944-1344</identifier><identifier>EISSN: 1614-7499</identifier><identifier>DOI: 10.1007/s11356-023-30811-2</identifier><identifier>PMID: 37957494</identifier><language>eng</language><publisher>Berlin/Heidelberg: Springer Berlin Heidelberg</publisher><subject>Air-water interface ; Aquatic Pollution ; Atmospheric Protection/Air Quality Control/Air Pollution ; Colloiding ; Continuum modeling ; Earth and Environmental Science ; Ecotoxicology ; Environment ; Environmental Chemistry ; Environmental Health ; Experiments ; Interfaces ; Leaching ; Lysimeters ; Mathematical models ; Parameters ; Particle tracking ; Perfluoroalkyl & polyfluoroalkyl substances ; Perfluorochemicals ; Precursors ; Random walk ; Research Article ; Retention ; Solid phases ; Sorption ; Transformations (mathematics) ; Waste Water Technology ; Water Management ; Water Pollution Control</subject><ispartof>Environmental science and pollution research international, 2023-12, Vol.30 (58), p.121529-121547</ispartof><rights>The Author(s) 2023</rights><rights>2023. The Author(s).</rights><rights>The Author(s) 2023. This work is published under http://creativecommons.org/licenses/by/4.0/ (the “License”). Notwithstanding the ProQuest Terms and Conditions, you may use this content in accordance with the terms of the License.</rights><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed><cites>FETCH-LOGICAL-c426t-3117bb2104c97a6743a347232a8febd4537a4c4cf9d189c41c3c89cd38439b093</cites><orcidid>0009-0002-2933-7048</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://link.springer.com/content/pdf/10.1007/s11356-023-30811-2$$EPDF$$P50$$Gspringer$$Hfree_for_read</linktopdf><linktohtml>$$Uhttps://link.springer.com/10.1007/s11356-023-30811-2$$EHTML$$P50$$Gspringer$$Hfree_for_read</linktohtml><link.rule.ids>230,314,780,784,885,27924,27925,41488,42557,51319</link.rule.ids><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/37957494$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink></links><search><creatorcontrib>Bierbaum, Thomas</creatorcontrib><creatorcontrib>Hansen, Scott K.</creatorcontrib><creatorcontrib>Poudel, Bikash</creatorcontrib><creatorcontrib>Haslauer, Claus</creatorcontrib><title>Investigating rate-limited sorption, sorption to air–water interfaces, and colloid-facilitated transport during PFAS leaching</title><title>Environmental science and pollution research international</title><addtitle>Environ Sci Pollut Res</addtitle><addtitle>Environ Sci Pollut Res Int</addtitle><description>Various sorption processes affect leaching of per- and polyfluoroalkyl substances (PFAS) such as PFOA and PFOS. The objectives of this study are to (1) compare rate-limited leaching in column and lysimeter experiments, (2) investigate the relevance of sorption to air–water interfaces (AWI), and (3) examine colloid-facilitated transport as a process explaining early experimental breakthrough. A continuum model (CM) with two-domain sorption is used to simulate equilibrium and rate-limited sorption. A random walk particle tracking (PT) model was developed and applied to analyze complex leaching characteristics. Results show that sorption parameters derived from column experiments underestimate long-term PFOA leaching in lysimeter experiments due to early depletion, suggesting that transformation of precursors contributes to the observed long-term leaching in the lysimeters (approximately 0.003 µg/kg/d PFOA). Both models demonstrate that sorption to AWI is the dominant retention mechanism for PFOS in lysimeter experiments, with retardation due to AWI being 3 (CM) to 3.7 (PT) times higher than retardation due to solid phase sorption. Notably, despite a simplified conception of AWI sorption, the PT results are closer to the observations. The PT simulations demonstrate possible colloid-facilitated transport at early time; however, results using substance-specific varying transport parameters align better with the observations, which should be equal if colloid-facilitated transport without additional kinetics is the sole mechanism affecting early breakthrough. Possibly, rate-limited sorption to AWI is relevant during the early stages of the lysimeter experiment. Our findings demonstrate that rate-limited sorption is less relevant for long-term leaching under field conditions compared to transformation of precursors and that sorption to AWI can be the dominant retention mechanism on contaminated sites. Moreover, they highlight the potential of random walk particle tracking as a practical alternative to continuum models for estimating the relative contributions of various retention mechanisms.</description><subject>Air-water interface</subject><subject>Aquatic Pollution</subject><subject>Atmospheric Protection/Air Quality Control/Air Pollution</subject><subject>Colloiding</subject><subject>Continuum modeling</subject><subject>Earth and Environmental Science</subject><subject>Ecotoxicology</subject><subject>Environment</subject><subject>Environmental Chemistry</subject><subject>Environmental Health</subject><subject>Experiments</subject><subject>Interfaces</subject><subject>Leaching</subject><subject>Lysimeters</subject><subject>Mathematical models</subject><subject>Parameters</subject><subject>Particle tracking</subject><subject>Perfluoroalkyl & polyfluoroalkyl substances</subject><subject>Perfluorochemicals</subject><subject>Precursors</subject><subject>Random 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Basic</collection><collection>MEDLINE - Academic</collection><collection>PubMed Central (Full Participant titles)</collection><jtitle>Environmental science and pollution research international</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Bierbaum, Thomas</au><au>Hansen, Scott K.</au><au>Poudel, Bikash</au><au>Haslauer, Claus</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Investigating rate-limited sorption, sorption to air–water interfaces, and colloid-facilitated transport during PFAS leaching</atitle><jtitle>Environmental science and pollution research international</jtitle><stitle>Environ Sci Pollut Res</stitle><addtitle>Environ Sci Pollut Res Int</addtitle><date>2023-12-01</date><risdate>2023</risdate><volume>30</volume><issue>58</issue><spage>121529</spage><epage>121547</epage><pages>121529-121547</pages><issn>1614-7499</issn><issn>0944-1344</issn><eissn>1614-7499</eissn><abstract>Various sorption processes affect leaching of per- and polyfluoroalkyl substances (PFAS) such as PFOA and PFOS. The objectives of this study are to (1) compare rate-limited leaching in column and lysimeter experiments, (2) investigate the relevance of sorption to air–water interfaces (AWI), and (3) examine colloid-facilitated transport as a process explaining early experimental breakthrough. A continuum model (CM) with two-domain sorption is used to simulate equilibrium and rate-limited sorption. A random walk particle tracking (PT) model was developed and applied to analyze complex leaching characteristics. Results show that sorption parameters derived from column experiments underestimate long-term PFOA leaching in lysimeter experiments due to early depletion, suggesting that transformation of precursors contributes to the observed long-term leaching in the lysimeters (approximately 0.003 µg/kg/d PFOA). Both models demonstrate that sorption to AWI is the dominant retention mechanism for PFOS in lysimeter experiments, with retardation due to AWI being 3 (CM) to 3.7 (PT) times higher than retardation due to solid phase sorption. Notably, despite a simplified conception of AWI sorption, the PT results are closer to the observations. The PT simulations demonstrate possible colloid-facilitated transport at early time; however, results using substance-specific varying transport parameters align better with the observations, which should be equal if colloid-facilitated transport without additional kinetics is the sole mechanism affecting early breakthrough. Possibly, rate-limited sorption to AWI is relevant during the early stages of the lysimeter experiment. Our findings demonstrate that rate-limited sorption is less relevant for long-term leaching under field conditions compared to transformation of precursors and that sorption to AWI can be the dominant retention mechanism on contaminated sites. Moreover, they highlight the potential of random walk particle tracking as a practical alternative to continuum models for estimating the relative contributions of various retention mechanisms.</abstract><cop>Berlin/Heidelberg</cop><pub>Springer Berlin Heidelberg</pub><pmid>37957494</pmid><doi>10.1007/s11356-023-30811-2</doi><tpages>19</tpages><orcidid>https://orcid.org/0009-0002-2933-7048</orcidid><oa>free_for_read</oa></addata></record> |
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subjects | Air-water interface Aquatic Pollution Atmospheric Protection/Air Quality Control/Air Pollution Colloiding Continuum modeling Earth and Environmental Science Ecotoxicology Environment Environmental Chemistry Environmental Health Experiments Interfaces Leaching Lysimeters Mathematical models Parameters Particle tracking Perfluoroalkyl & polyfluoroalkyl substances Perfluorochemicals Precursors Random walk Research Article Retention Solid phases Sorption Transformations (mathematics) Waste Water Technology Water Management Water Pollution Control |
title | Investigating rate-limited sorption, sorption to air–water interfaces, and colloid-facilitated transport during PFAS leaching |
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