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Uranium(VI) Adsorption and Surface Complexation Modeling onto Background Sediments from the F-Area Savannah River Site
The mobility of an acidic uranium waste plume in the F-Area of Savannah River Site is of great concern. In order to understand and predict uranium mobility, U(VI) adsorption experiments were performed as a function of pH using background F-Area aquifer sediments and reference goethite and kaolinite...
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Published in: | Environmental science & technology 2012-02, Vol.46 (3), p.1565-1571 |
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description | The mobility of an acidic uranium waste plume in the F-Area of Savannah River Site is of great concern. In order to understand and predict uranium mobility, U(VI) adsorption experiments were performed as a function of pH using background F-Area aquifer sediments and reference goethite and kaolinite (major reactive phases of F-Area sediments), and a component-additivity (CA) based surface complexation model (SCM) was developed. Our experimental results indicate that the fine fractions (≤45 μm) in sediments control U(VI) adsorption due to their large surface area, although the quartz sands show a stronger adsorption ability per unit surface area than the fine fractions at pH < 5.0. Kaolinite is a more important sorbent for U(VI) at pH < 4.0, while goethite plays a major role at pH > 4.0. Our CA model combines an existing U(VI) SCM for goethite and a modified U(VI) SCM for kaolinite along with estimated relative surface area abundances of these component minerals. The modeling approach successfully predicts U(VI) adsorption behavior by the background F-Area sediments. The model suggests that exchange sites on kaolinite dominate U(VI) adsorption at pH < 4.0, goethite and kaolinite edge sites cocontribute to U(VI) adsorption at pH 4.0–6.0, and goethite dominates U(VI) adsorption at pH > 6.0. |
doi_str_mv | 10.1021/es2036256 |
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In order to understand and predict uranium mobility, U(VI) adsorption experiments were performed as a function of pH using background F-Area aquifer sediments and reference goethite and kaolinite (major reactive phases of F-Area sediments), and a component-additivity (CA) based surface complexation model (SCM) was developed. Our experimental results indicate that the fine fractions (≤45 μm) in sediments control U(VI) adsorption due to their large surface area, although the quartz sands show a stronger adsorption ability per unit surface area than the fine fractions at pH < 5.0. Kaolinite is a more important sorbent for U(VI) at pH < 4.0, while goethite plays a major role at pH > 4.0. Our CA model combines an existing U(VI) SCM for goethite and a modified U(VI) SCM for kaolinite along with estimated relative surface area abundances of these component minerals. The modeling approach successfully predicts U(VI) adsorption behavior by the background F-Area sediments. The model suggests that exchange sites on kaolinite dominate U(VI) adsorption at pH < 4.0, goethite and kaolinite edge sites cocontribute to U(VI) adsorption at pH 4.0–6.0, and goethite dominates U(VI) adsorption at pH > 6.0.</description><identifier>ISSN: 0013-936X</identifier><identifier>EISSN: 1520-5851</identifier><identifier>DOI: 10.1021/es2036256</identifier><identifier>PMID: 22191402</identifier><identifier>CODEN: ESTHAG</identifier><language>eng</language><publisher>Washington, DC: American Chemical Society</publisher><subject>Adsorption ; Applied sciences ; Aquifers ; Biological and physicochemical properties of pollutants. Interaction in the soil ; Earth sciences ; Earth, ocean, space ; Engineering and environment geology. Geothermics ; Exact sciences and technology ; Geologic Sediments - chemistry ; Georgia ; Groundwater - chemistry ; Groundwaters ; Hydrogen-Ion Concentration ; Iron Compounds - chemistry ; Kaolin - chemistry ; Minerals ; Minerals - chemistry ; Models, Chemical ; Natural water pollution ; Pollution ; Pollution, environment geology ; Quartz - chemistry ; Radioactive Pollutants - analysis ; Radioactive Pollutants - chemistry ; Rivers ; Sediments ; Soil and sediments pollution ; Uranium ; Uranium - analysis ; Uranium - chemistry ; Water treatment and pollution</subject><ispartof>Environmental science & technology, 2012-02, Vol.46 (3), p.1565-1571</ispartof><rights>Copyright © 2011 American Chemical Society</rights><rights>2014 INIST-CNRS</rights><rights>Copyright American Chemical Society Feb 7, 2012</rights><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-a499t-181e5d14d119d313c2ffcb3c71b132de8d2639055fe73d7c100eef87d7f2bca83</citedby><cites>FETCH-LOGICAL-a499t-181e5d14d119d313c2ffcb3c71b132de8d2639055fe73d7c100eef87d7f2bca83</cites></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><link.rule.ids>230,314,776,780,881,27901,27902</link.rule.ids><backlink>$$Uhttp://pascal-francis.inist.fr/vibad/index.php?action=getRecordDetail&idt=25630590$$DView record in Pascal Francis$$Hfree_for_read</backlink><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/22191402$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink><backlink>$$Uhttps://www.osti.gov/biblio/1154340$$D View this record in Osti.gov$$Hfree_for_read</backlink></links><search><creatorcontrib>Dong, Wenming</creatorcontrib><creatorcontrib>Tokunaga, Tetsu K</creatorcontrib><creatorcontrib>Davis, James A</creatorcontrib><creatorcontrib>Wan, Jiamin</creatorcontrib><creatorcontrib>Subsurface Biogeochemical Research (SBR)</creatorcontrib><title>Uranium(VI) Adsorption and Surface Complexation Modeling onto Background Sediments from the F-Area Savannah River Site</title><title>Environmental science & technology</title><addtitle>Environ. Sci. Technol</addtitle><description>The mobility of an acidic uranium waste plume in the F-Area of Savannah River Site is of great concern. In order to understand and predict uranium mobility, U(VI) adsorption experiments were performed as a function of pH using background F-Area aquifer sediments and reference goethite and kaolinite (major reactive phases of F-Area sediments), and a component-additivity (CA) based surface complexation model (SCM) was developed. Our experimental results indicate that the fine fractions (≤45 μm) in sediments control U(VI) adsorption due to their large surface area, although the quartz sands show a stronger adsorption ability per unit surface area than the fine fractions at pH < 5.0. Kaolinite is a more important sorbent for U(VI) at pH < 4.0, while goethite plays a major role at pH > 4.0. Our CA model combines an existing U(VI) SCM for goethite and a modified U(VI) SCM for kaolinite along with estimated relative surface area abundances of these component minerals. The modeling approach successfully predicts U(VI) adsorption behavior by the background F-Area sediments. The model suggests that exchange sites on kaolinite dominate U(VI) adsorption at pH < 4.0, goethite and kaolinite edge sites cocontribute to U(VI) adsorption at pH 4.0–6.0, and goethite dominates U(VI) adsorption at pH > 6.0.</description><subject>Adsorption</subject><subject>Applied sciences</subject><subject>Aquifers</subject><subject>Biological and physicochemical properties of pollutants. Interaction in the soil</subject><subject>Earth sciences</subject><subject>Earth, ocean, space</subject><subject>Engineering and environment geology. Geothermics</subject><subject>Exact sciences and technology</subject><subject>Geologic Sediments - chemistry</subject><subject>Georgia</subject><subject>Groundwater - chemistry</subject><subject>Groundwaters</subject><subject>Hydrogen-Ion Concentration</subject><subject>Iron Compounds - chemistry</subject><subject>Kaolin - chemistry</subject><subject>Minerals</subject><subject>Minerals - chemistry</subject><subject>Models, Chemical</subject><subject>Natural water pollution</subject><subject>Pollution</subject><subject>Pollution, environment geology</subject><subject>Quartz - chemistry</subject><subject>Radioactive Pollutants - analysis</subject><subject>Radioactive Pollutants - chemistry</subject><subject>Rivers</subject><subject>Sediments</subject><subject>Soil and sediments pollution</subject><subject>Uranium</subject><subject>Uranium - analysis</subject><subject>Uranium - chemistry</subject><subject>Water treatment and pollution</subject><issn>0013-936X</issn><issn>1520-5851</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2012</creationdate><recordtype>article</recordtype><recordid>eNpl0UFv0zAUB3ALMbEyOPAFkIWE2A4BPztukmOp2Jg0hEQZ4ha59vPqkdidnVTw7XFp1x44-eCf_u_Zf0JeAXsPjMMHTJyJKZfTJ2QCkrNC1hKekgljIIpGTH-ekucp3TPGuGD1M3LKOTRQMj4hm9uovBv78x_XF3RmUojrwQVPlTd0MUarNNJ56Ncd_lb_Lr4Eg53zdzT4IdCPSv-6i2HcajSuRz8kamPo6bBCelnMIiq6UBvlvVrRb26DkS7cgC_IiVVdwpf784zcXn76Pv9c3Hy9up7PbgpVNs1QQA0oDZQGoDEChObW6qXQFSxBcIO14VPRMCktVsJUGhhDtHVlKsuXWtXijLzZ5YY0uDbpPFqvdPAe9dACyFKULKN3O7SO4WHENLS9Sxq7TnkMY2qb7e9WpayOcQd5H8bo8wsy4lLmfZuMLnZIx5BSRNuuo-tV_NMCa7d9tYe-sn29DxyXPZqDfCwog7d7oJJWnc1taZeOLmcw2bCjUzodl_p_4F84tKdu</recordid><startdate>20120207</startdate><enddate>20120207</enddate><creator>Dong, Wenming</creator><creator>Tokunaga, Tetsu K</creator><creator>Davis, James A</creator><creator>Wan, Jiamin</creator><general>American Chemical Society</general><scope>IQODW</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>7QO</scope><scope>7ST</scope><scope>7T7</scope><scope>7U7</scope><scope>8FD</scope><scope>C1K</scope><scope>FR3</scope><scope>P64</scope><scope>SOI</scope><scope>7X8</scope><scope>OTOTI</scope></search><sort><creationdate>20120207</creationdate><title>Uranium(VI) Adsorption and Surface Complexation Modeling onto Background Sediments from the F-Area Savannah River Site</title><author>Dong, Wenming ; Tokunaga, Tetsu K ; Davis, James A ; Wan, Jiamin</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-a499t-181e5d14d119d313c2ffcb3c71b132de8d2639055fe73d7c100eef87d7f2bca83</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2012</creationdate><topic>Adsorption</topic><topic>Applied sciences</topic><topic>Aquifers</topic><topic>Biological and physicochemical properties of pollutants. Interaction in the soil</topic><topic>Earth sciences</topic><topic>Earth, ocean, space</topic><topic>Engineering and environment geology. Geothermics</topic><topic>Exact sciences and technology</topic><topic>Geologic Sediments - chemistry</topic><topic>Georgia</topic><topic>Groundwater - chemistry</topic><topic>Groundwaters</topic><topic>Hydrogen-Ion Concentration</topic><topic>Iron Compounds - chemistry</topic><topic>Kaolin - chemistry</topic><topic>Minerals</topic><topic>Minerals - chemistry</topic><topic>Models, Chemical</topic><topic>Natural water pollution</topic><topic>Pollution</topic><topic>Pollution, environment geology</topic><topic>Quartz - chemistry</topic><topic>Radioactive Pollutants - analysis</topic><topic>Radioactive Pollutants - chemistry</topic><topic>Rivers</topic><topic>Sediments</topic><topic>Soil and sediments pollution</topic><topic>Uranium</topic><topic>Uranium - analysis</topic><topic>Uranium - chemistry</topic><topic>Water treatment and pollution</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Dong, Wenming</creatorcontrib><creatorcontrib>Tokunaga, Tetsu K</creatorcontrib><creatorcontrib>Davis, James A</creatorcontrib><creatorcontrib>Wan, Jiamin</creatorcontrib><creatorcontrib>Subsurface Biogeochemical Research (SBR)</creatorcontrib><collection>Pascal-Francis</collection><collection>Medline</collection><collection>MEDLINE</collection><collection>MEDLINE (Ovid)</collection><collection>MEDLINE</collection><collection>MEDLINE</collection><collection>PubMed</collection><collection>CrossRef</collection><collection>Biotechnology Research Abstracts</collection><collection>Environment Abstracts</collection><collection>Industrial and Applied Microbiology Abstracts (Microbiology A)</collection><collection>Toxicology Abstracts</collection><collection>Technology Research Database</collection><collection>Environmental Sciences and Pollution Management</collection><collection>Engineering Research Database</collection><collection>Biotechnology and BioEngineering Abstracts</collection><collection>Environment Abstracts</collection><collection>MEDLINE - Academic</collection><collection>OSTI.GOV</collection><jtitle>Environmental science & technology</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Dong, Wenming</au><au>Tokunaga, Tetsu K</au><au>Davis, James A</au><au>Wan, Jiamin</au><aucorp>Subsurface Biogeochemical Research (SBR)</aucorp><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Uranium(VI) Adsorption and Surface Complexation Modeling onto Background Sediments from the F-Area Savannah River Site</atitle><jtitle>Environmental science & technology</jtitle><addtitle>Environ. Sci. Technol</addtitle><date>2012-02-07</date><risdate>2012</risdate><volume>46</volume><issue>3</issue><spage>1565</spage><epage>1571</epage><pages>1565-1571</pages><issn>0013-936X</issn><eissn>1520-5851</eissn><coden>ESTHAG</coden><abstract>The mobility of an acidic uranium waste plume in the F-Area of Savannah River Site is of great concern. In order to understand and predict uranium mobility, U(VI) adsorption experiments were performed as a function of pH using background F-Area aquifer sediments and reference goethite and kaolinite (major reactive phases of F-Area sediments), and a component-additivity (CA) based surface complexation model (SCM) was developed. Our experimental results indicate that the fine fractions (≤45 μm) in sediments control U(VI) adsorption due to their large surface area, although the quartz sands show a stronger adsorption ability per unit surface area than the fine fractions at pH < 5.0. Kaolinite is a more important sorbent for U(VI) at pH < 4.0, while goethite plays a major role at pH > 4.0. Our CA model combines an existing U(VI) SCM for goethite and a modified U(VI) SCM for kaolinite along with estimated relative surface area abundances of these component minerals. The modeling approach successfully predicts U(VI) adsorption behavior by the background F-Area sediments. The model suggests that exchange sites on kaolinite dominate U(VI) adsorption at pH < 4.0, goethite and kaolinite edge sites cocontribute to U(VI) adsorption at pH 4.0–6.0, and goethite dominates U(VI) adsorption at pH > 6.0.</abstract><cop>Washington, DC</cop><pub>American Chemical Society</pub><pmid>22191402</pmid><doi>10.1021/es2036256</doi><tpages>7</tpages><oa>free_for_read</oa></addata></record> |
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subjects | Adsorption Applied sciences Aquifers Biological and physicochemical properties of pollutants. Interaction in the soil Earth sciences Earth, ocean, space Engineering and environment geology. Geothermics Exact sciences and technology Geologic Sediments - chemistry Georgia Groundwater - chemistry Groundwaters Hydrogen-Ion Concentration Iron Compounds - chemistry Kaolin - chemistry Minerals Minerals - chemistry Models, Chemical Natural water pollution Pollution Pollution, environment geology Quartz - chemistry Radioactive Pollutants - analysis Radioactive Pollutants - chemistry Rivers Sediments Soil and sediments pollution Uranium Uranium - analysis Uranium - chemistry Water treatment and pollution |
title | Uranium(VI) Adsorption and Surface Complexation Modeling onto Background Sediments from the F-Area Savannah River Site |
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