Elucidating mobilization mechanisms of uranium during recharge of river water to contaminated groundwater
The recharge of stream water below the baseflow water table can mobilize groundwater contaminants, particularly redox-sensitive and sorptive metals such as uranium. However, in-situ tracer experiments that simulate the recharge of stream water to uranium-contaminated groundwater are lacking, thus li...
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Veröffentlicht in: | Journal of contaminant hydrology 2022-12, Vol.251 (C), p.104076, Article 104076 |
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creator | Paradis, Charles J. Hoss, Kendyl N. Meurer, Cullen E. Hatami, Jiyan L. Dangelmayr, Martin A. Tigar, Aaron D. Johnson, Raymond H. |
description | The recharge of stream water below the baseflow water table can mobilize groundwater contaminants, particularly redox-sensitive and sorptive metals such as uranium. However, in-situ tracer experiments that simulate the recharge of stream water to uranium-contaminated groundwater are lacking, thus limiting the understanding of the potential mechanisms that control the mobility of uranium at the field scale. In this study, a field tracer test was conducted by injecting 100 gal (379 l) of oxic river water into a nearby suboxic and uranium-contaminated aquifer. The traced river water was monitored for 18 days in the single injection well and in the twelve surrounding observation wells. Mobilization of uranium from the solid to the aqueous phase was not observed during the tracer test despite its pre-test presence being confirmed on the aquifer sediments from lab-based acid leaching. However, strong evidence of oxidative immobilization of iron and manganese was observed during the tracer test and suggested that immobile uranium was likely in its oxidized state as U(VI) on the aquifer sediments; these observations ruled out oxidation of U(IV) to U(VI) as a potential mobilization mechanism. Therefore, desorption of U(VI) appeared to be the predominant potential mobilization mechanism, yet it was clearly not solely dependent on concentration as evident when considering that uranium-poor river water ( |
doi_str_mv | 10.1016/j.jconhyd.2022.104076 |
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•Surface water to groundwater recharge can mobilize aquifer contaminants.•Field tracer test injected clean river water to uranium-contaminated groundwater.•Uranium mobilization dominated by advection, dispersion, and dilution.•Uranium dissolution and/or desorption not observed, but might be very slow.•Future studies should focus on uranium mobilization above water table.</description><identifier>ISSN: 0169-7722</identifier><identifier>EISSN: 1873-6009</identifier><identifier>DOI: 10.1016/j.jconhyd.2022.104076</identifier><identifier>PMID: 36148719</identifier><language>eng</language><publisher>Netherlands: Elsevier B.V</publisher><subject>Desorption ; Dissolution ; Geologic Sediments ; Groundwater ; Minerals ; Rivers ; Surface water ; Tracer ; Uranium ; Uranium - analysis ; Water ; Water Pollutants, Radioactive - analysis</subject><ispartof>Journal of contaminant hydrology, 2022-12, Vol.251 (C), p.104076, Article 104076</ispartof><rights>2022 The Authors</rights><rights>Copyright © 2022 The Authors. Published by Elsevier B.V. All rights reserved.</rights><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-a462t-a8e96508d7913088437ebd8b486431df08d1f45491e1385b47a6c7270e9c13173</citedby><cites>FETCH-LOGICAL-a462t-a8e96508d7913088437ebd8b486431df08d1f45491e1385b47a6c7270e9c13173</cites></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktohtml>$$Uhttps://dx.doi.org/10.1016/j.jconhyd.2022.104076$$EHTML$$P50$$Gelsevier$$Hfree_for_read</linktohtml><link.rule.ids>230,315,781,785,886,3551,27929,27930,46000</link.rule.ids><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/36148719$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink><backlink>$$Uhttps://www.osti.gov/biblio/1889326$$D View this record in Osti.gov$$Hfree_for_read</backlink></links><search><creatorcontrib>Paradis, Charles J.</creatorcontrib><creatorcontrib>Hoss, Kendyl N.</creatorcontrib><creatorcontrib>Meurer, Cullen E.</creatorcontrib><creatorcontrib>Hatami, Jiyan L.</creatorcontrib><creatorcontrib>Dangelmayr, Martin A.</creatorcontrib><creatorcontrib>Tigar, Aaron D.</creatorcontrib><creatorcontrib>Johnson, Raymond H.</creatorcontrib><title>Elucidating mobilization mechanisms of uranium during recharge of river water to contaminated groundwater</title><title>Journal of contaminant hydrology</title><addtitle>J Contam Hydrol</addtitle><description>The recharge of stream water below the baseflow water table can mobilize groundwater contaminants, particularly redox-sensitive and sorptive metals such as uranium. However, in-situ tracer experiments that simulate the recharge of stream water to uranium-contaminated groundwater are lacking, thus limiting the understanding of the potential mechanisms that control the mobility of uranium at the field scale. In this study, a field tracer test was conducted by injecting 100 gal (379 l) of oxic river water into a nearby suboxic and uranium-contaminated aquifer. The traced river water was monitored for 18 days in the single injection well and in the twelve surrounding observation wells. Mobilization of uranium from the solid to the aqueous phase was not observed during the tracer test despite its pre-test presence being confirmed on the aquifer sediments from lab-based acid leaching. However, strong evidence of oxidative immobilization of iron and manganese was observed during the tracer test and suggested that immobile uranium was likely in its oxidized state as U(VI) on the aquifer sediments; these observations ruled out oxidation of U(IV) to U(VI) as a potential mobilization mechanism. Therefore, desorption of U(VI) appeared to be the predominant potential mobilization mechanism, yet it was clearly not solely dependent on concentration as evident when considering that uranium-poor river water (<0.015 mg/L) was recharged to uranium-rich groundwater (≈1 mg/L). It was possible that uranium desorption was limited by the relatively higher pH and lower alkalinity of the river water as compared to the groundwater; both factors favor immobilization. However, it was likely that the immobile uranium was associated with a mineral phase, as opposed to a sorbed phase, thus desorption may not have been possible. The results of this field tracer study successfully ruled out two common mobilization mechanisms of uranium: (1) oxidative dissolution and (2) concentration-dependent desorption and ruled in the importance of advection, dispersion, and the mineral phase of uranium.
•Surface water to groundwater recharge can mobilize aquifer contaminants.•Field tracer test injected clean river water to uranium-contaminated groundwater.•Uranium mobilization dominated by advection, dispersion, and dilution.•Uranium dissolution and/or desorption not observed, but might be very slow.•Future studies should focus on uranium mobilization above water table.</description><subject>Desorption</subject><subject>Dissolution</subject><subject>Geologic Sediments</subject><subject>Groundwater</subject><subject>Minerals</subject><subject>Rivers</subject><subject>Surface water</subject><subject>Tracer</subject><subject>Uranium</subject><subject>Uranium - analysis</subject><subject>Water</subject><subject>Water Pollutants, Radioactive - analysis</subject><issn>0169-7722</issn><issn>1873-6009</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2022</creationdate><recordtype>article</recordtype><sourceid>EIF</sourceid><recordid>eNqFkF1PwyAUhonRuDn9CZrG-04olI8rY5b5kSzxRq8JBbqxrGWBdkZ_vdROb70BDu9zDi8vANcIzhFE9G4732rfbj7NvIBFke4IZPQETBFnOKcQilMwTZzIGSuKCbiIcQshZBzyczDBFBHOkJgCt9z12hnVuXadNb5yO_eVCt9mjdUb1brYxMzXWR_SuW8y04eBDIMY1naQgjvYkH2oLq2dz5KrTjWuTbXJ1sH3rfnRLsFZrXbRXh33GXh_XL4tnvPV69PL4mGVK0KLLlfcClpCbphAGHJOMLOV4RXhlGBk6qSgmpREIIswLyvCFNWsYNAKjTBieAZux7k-dk5G7brkNZlqre4k4lzggiaoHCEdfIzB1nIfXKPCp0RQDvnKrTzmK4d85Zhv6rsZ-_Z91Vjz1_UbaALuR8CmLx6cDYMD22prXBgMGO_-eeIbRKaPlw</recordid><startdate>202212</startdate><enddate>202212</enddate><creator>Paradis, Charles J.</creator><creator>Hoss, Kendyl N.</creator><creator>Meurer, Cullen E.</creator><creator>Hatami, Jiyan L.</creator><creator>Dangelmayr, Martin A.</creator><creator>Tigar, Aaron D.</creator><creator>Johnson, Raymond H.</creator><general>Elsevier B.V</general><general>Elsevier</general><scope>6I.</scope><scope>AAFTH</scope><scope>CGR</scope><scope>CUY</scope><scope>CVF</scope><scope>ECM</scope><scope>EIF</scope><scope>NPM</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>OTOTI</scope></search><sort><creationdate>202212</creationdate><title>Elucidating mobilization mechanisms of uranium during recharge of river water to contaminated groundwater</title><author>Paradis, Charles J. ; Hoss, Kendyl N. ; Meurer, Cullen E. ; Hatami, Jiyan L. ; Dangelmayr, Martin A. ; Tigar, Aaron D. ; Johnson, Raymond H.</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-a462t-a8e96508d7913088437ebd8b486431df08d1f45491e1385b47a6c7270e9c13173</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2022</creationdate><topic>Desorption</topic><topic>Dissolution</topic><topic>Geologic Sediments</topic><topic>Groundwater</topic><topic>Minerals</topic><topic>Rivers</topic><topic>Surface water</topic><topic>Tracer</topic><topic>Uranium</topic><topic>Uranium - analysis</topic><topic>Water</topic><topic>Water Pollutants, Radioactive - analysis</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Paradis, Charles J.</creatorcontrib><creatorcontrib>Hoss, Kendyl N.</creatorcontrib><creatorcontrib>Meurer, Cullen E.</creatorcontrib><creatorcontrib>Hatami, Jiyan L.</creatorcontrib><creatorcontrib>Dangelmayr, Martin A.</creatorcontrib><creatorcontrib>Tigar, Aaron D.</creatorcontrib><creatorcontrib>Johnson, Raymond H.</creatorcontrib><collection>ScienceDirect Open Access Titles</collection><collection>Elsevier:ScienceDirect:Open Access</collection><collection>Medline</collection><collection>MEDLINE</collection><collection>MEDLINE (Ovid)</collection><collection>MEDLINE</collection><collection>MEDLINE</collection><collection>PubMed</collection><collection>CrossRef</collection><collection>OSTI.GOV</collection><jtitle>Journal of contaminant hydrology</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Paradis, Charles J.</au><au>Hoss, Kendyl N.</au><au>Meurer, Cullen E.</au><au>Hatami, Jiyan L.</au><au>Dangelmayr, Martin A.</au><au>Tigar, Aaron D.</au><au>Johnson, Raymond H.</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Elucidating mobilization mechanisms of uranium during recharge of river water to contaminated groundwater</atitle><jtitle>Journal of contaminant hydrology</jtitle><addtitle>J Contam Hydrol</addtitle><date>2022-12</date><risdate>2022</risdate><volume>251</volume><issue>C</issue><spage>104076</spage><pages>104076-</pages><artnum>104076</artnum><issn>0169-7722</issn><eissn>1873-6009</eissn><abstract>The recharge of stream water below the baseflow water table can mobilize groundwater contaminants, particularly redox-sensitive and sorptive metals such as uranium. However, in-situ tracer experiments that simulate the recharge of stream water to uranium-contaminated groundwater are lacking, thus limiting the understanding of the potential mechanisms that control the mobility of uranium at the field scale. In this study, a field tracer test was conducted by injecting 100 gal (379 l) of oxic river water into a nearby suboxic and uranium-contaminated aquifer. The traced river water was monitored for 18 days in the single injection well and in the twelve surrounding observation wells. Mobilization of uranium from the solid to the aqueous phase was not observed during the tracer test despite its pre-test presence being confirmed on the aquifer sediments from lab-based acid leaching. However, strong evidence of oxidative immobilization of iron and manganese was observed during the tracer test and suggested that immobile uranium was likely in its oxidized state as U(VI) on the aquifer sediments; these observations ruled out oxidation of U(IV) to U(VI) as a potential mobilization mechanism. Therefore, desorption of U(VI) appeared to be the predominant potential mobilization mechanism, yet it was clearly not solely dependent on concentration as evident when considering that uranium-poor river water (<0.015 mg/L) was recharged to uranium-rich groundwater (≈1 mg/L). It was possible that uranium desorption was limited by the relatively higher pH and lower alkalinity of the river water as compared to the groundwater; both factors favor immobilization. However, it was likely that the immobile uranium was associated with a mineral phase, as opposed to a sorbed phase, thus desorption may not have been possible. The results of this field tracer study successfully ruled out two common mobilization mechanisms of uranium: (1) oxidative dissolution and (2) concentration-dependent desorption and ruled in the importance of advection, dispersion, and the mineral phase of uranium.
•Surface water to groundwater recharge can mobilize aquifer contaminants.•Field tracer test injected clean river water to uranium-contaminated groundwater.•Uranium mobilization dominated by advection, dispersion, and dilution.•Uranium dissolution and/or desorption not observed, but might be very slow.•Future studies should focus on uranium mobilization above water table.</abstract><cop>Netherlands</cop><pub>Elsevier B.V</pub><pmid>36148719</pmid><doi>10.1016/j.jconhyd.2022.104076</doi><oa>free_for_read</oa></addata></record> |
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source | MEDLINE; ScienceDirect Journals (5 years ago - present) |
subjects | Desorption Dissolution Geologic Sediments Groundwater Minerals Rivers Surface water Tracer Uranium Uranium - analysis Water Water Pollutants, Radioactive - analysis |
title | Elucidating mobilization mechanisms of uranium during recharge of river water to contaminated groundwater |
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