The effect of EDTA on the groundwater transport of thorium through sand

The effect of the anthropogenic complexing agent EDTA on thorium transport in groundwater has been studied using sand-packed columns and flow rates in the range of 20–100 m y−1. The concentrations injected into the columns were in the range of 0.4–4 mM for Th and 4–40 mM for EDTA, and with EDTA:Th r...

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Veröffentlicht in:Water research (Oxford) 2012-10, Vol.46 (15), p.4870-4882
Hauptverfasser: May, Colin C., Young, Lindsay, Worsfold, Paul J., Heath, Sarah, Bryan, Nick D., Keith-Roach, Miranda J.
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container_end_page 4882
container_issue 15
container_start_page 4870
container_title Water research (Oxford)
container_volume 46
creator May, Colin C.
Young, Lindsay
Worsfold, Paul J.
Heath, Sarah
Bryan, Nick D.
Keith-Roach, Miranda J.
description The effect of the anthropogenic complexing agent EDTA on thorium transport in groundwater has been studied using sand-packed columns and flow rates in the range of 20–100 m y−1. The concentrations injected into the columns were in the range of 0.4–4 mM for Th and 4–40 mM for EDTA, and with EDTA:Th ratios in the range 1:1 to 10:1. The results show that EDTA can significantly increase Th transport, but two very different behaviours are observed at Th concentrations of 0.4 and 4 mM. At the lower concentration, Th breakthrough is retarded with respect to a conservative tracer, with a peak width that is consistent with a single Kd value, followed by a longer tail, and the behaviour is very sensitive to the flow rate. However at 4 mM Th, the breakthrough peak appears near to that of the tracer, and the width of the peak is consistent with a distribution of Kd values and/or a larger dispersivity than the tracer. Speciation and transport modelling have been used to interpret the data, and a model was developed that could explain the 0.4 mM behaviour. This suggests that ternary surface complexes are important in these systems, with at least two different species involved, although the complexity of Th speciation in these systems leads to significant uncertainty in the values of the equilibrium and kinetic parameters. For the 4 mM systems, the rapid transport observed could not be explained by a simple chemical model; instead it is likely that EDTA plays an important role in stabilising and transporting thorium colloids and clusters. [Display omitted] ► EDTA has been shown to enhance thorium migration through sand significantly. ► Transport involves ternary interactions between Th-EDTA complexes and the sand. ► The concentration of thorium and EDTA affects the transport mechanism. ► A simple chemical model has been developed to explain thorium behaviour at low concentrations. ► Evidence is provided for mobile EDTA-stabilised thorium colloidal transport at high thorium and EDTA concentrations.
doi_str_mv 10.1016/j.watres.2012.06.012
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The concentrations injected into the columns were in the range of 0.4–4 mM for Th and 4–40 mM for EDTA, and with EDTA:Th ratios in the range 1:1 to 10:1. The results show that EDTA can significantly increase Th transport, but two very different behaviours are observed at Th concentrations of 0.4 and 4 mM. At the lower concentration, Th breakthrough is retarded with respect to a conservative tracer, with a peak width that is consistent with a single Kd value, followed by a longer tail, and the behaviour is very sensitive to the flow rate. However at 4 mM Th, the breakthrough peak appears near to that of the tracer, and the width of the peak is consistent with a distribution of Kd values and/or a larger dispersivity than the tracer. Speciation and transport modelling have been used to interpret the data, and a model was developed that could explain the 0.4 mM behaviour. This suggests that ternary surface complexes are important in these systems, with at least two different species involved, although the complexity of Th speciation in these systems leads to significant uncertainty in the values of the equilibrium and kinetic parameters. For the 4 mM systems, the rapid transport observed could not be explained by a simple chemical model; instead it is likely that EDTA plays an important role in stabilising and transporting thorium colloids and clusters. [Display omitted] ► EDTA has been shown to enhance thorium migration through sand significantly. ► Transport involves ternary interactions between Th-EDTA complexes and the sand. ► The concentration of thorium and EDTA affects the transport mechanism. ► A simple chemical model has been developed to explain thorium behaviour at low concentrations. ► Evidence is provided for mobile EDTA-stabilised thorium colloidal transport at high thorium and EDTA concentrations.</description><identifier>ISSN: 0043-1354</identifier><identifier>EISSN: 1879-2448</identifier><identifier>DOI: 10.1016/j.watres.2012.06.012</identifier><identifier>PMID: 22796006</identifier><identifier>CODEN: WATRAG</identifier><language>eng</language><publisher>Kidlington: Elsevier Ltd</publisher><subject>Applied sciences ; Colloid ; colloids ; Complexation ; Complexing agent ; Edetic Acid - chemistry ; EDTA (chelating agent) ; Exact sciences and technology ; Groundwater - chemistry ; groundwater flow ; Migration ; Modelling ; Models, Theoretical ; Pollution ; sand ; Silicon Dioxide ; Speciation ; thorium ; Thorium - chemistry ; uncertainty ; Water treatment and pollution</subject><ispartof>Water research (Oxford), 2012-10, Vol.46 (15), p.4870-4882</ispartof><rights>2012 Elsevier Ltd</rights><rights>2015 INIST-CNRS</rights><rights>Copyright © 2012 Elsevier Ltd. 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The concentrations injected into the columns were in the range of 0.4–4 mM for Th and 4–40 mM for EDTA, and with EDTA:Th ratios in the range 1:1 to 10:1. The results show that EDTA can significantly increase Th transport, but two very different behaviours are observed at Th concentrations of 0.4 and 4 mM. At the lower concentration, Th breakthrough is retarded with respect to a conservative tracer, with a peak width that is consistent with a single Kd value, followed by a longer tail, and the behaviour is very sensitive to the flow rate. However at 4 mM Th, the breakthrough peak appears near to that of the tracer, and the width of the peak is consistent with a distribution of Kd values and/or a larger dispersivity than the tracer. Speciation and transport modelling have been used to interpret the data, and a model was developed that could explain the 0.4 mM behaviour. This suggests that ternary surface complexes are important in these systems, with at least two different species involved, although the complexity of Th speciation in these systems leads to significant uncertainty in the values of the equilibrium and kinetic parameters. For the 4 mM systems, the rapid transport observed could not be explained by a simple chemical model; instead it is likely that EDTA plays an important role in stabilising and transporting thorium colloids and clusters. [Display omitted] ► EDTA has been shown to enhance thorium migration through sand significantly. ► Transport involves ternary interactions between Th-EDTA complexes and the sand. ► The concentration of thorium and EDTA affects the transport mechanism. ► A simple chemical model has been developed to explain thorium behaviour at low concentrations. ► Evidence is provided for mobile EDTA-stabilised thorium colloidal transport at high thorium and EDTA concentrations.</description><subject>Applied sciences</subject><subject>Colloid</subject><subject>colloids</subject><subject>Complexation</subject><subject>Complexing agent</subject><subject>Edetic Acid - chemistry</subject><subject>EDTA (chelating agent)</subject><subject>Exact sciences and technology</subject><subject>Groundwater - chemistry</subject><subject>groundwater flow</subject><subject>Migration</subject><subject>Modelling</subject><subject>Models, Theoretical</subject><subject>Pollution</subject><subject>sand</subject><subject>Silicon Dioxide</subject><subject>Speciation</subject><subject>thorium</subject><subject>Thorium - chemistry</subject><subject>uncertainty</subject><subject>Water treatment and pollution</subject><issn>0043-1354</issn><issn>1879-2448</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2012</creationdate><recordtype>article</recordtype><sourceid>EIF</sourceid><recordid>eNp90ctq3DAUBmBRWppJ2jcIqTeFbOweXSxbm0JIcykEushkLWRdZjzMWFPJbsnb90w8aXdd_SC-oyN-EXJOoaJA5ZdN9duMyeeKAWUVyArjDVnQtlElE6J9SxYAgpeU1-KEnOa8AQDGuHpPThhrlASQC3K3XPvCh-DtWMRQ3HxbXhVxKEY8XaU4DQ6X-FSMyQx5H9MLGtcx9dMOE8VqXWQzuA_kXTDb7D8e84w83d4sr-_Lhx9336-vHkorqBxLV6vQda5pjaRC1kYIDq5j0FjWWh5o4HWwEljwLnDLnKwd80KAs065ujP8jFzO9-5T_Dn5POpdn63fbs3g45Q1BdbIlnGhkIqZ2hRzTj7ofep3Jj0j0ocK9UbPFepDhRqkxsCxi-OGqdt593fotTMEn4_AZGu2Aauxff7nJFWMtgf3aXbBRG1WCc3TI26q8R9AgRIovs7CY2O_ep90tr0frHd9wg_RLvb_f-sfyEiaHw</recordid><startdate>20121001</startdate><enddate>20121001</enddate><creator>May, Colin C.</creator><creator>Young, Lindsay</creator><creator>Worsfold, Paul J.</creator><creator>Heath, Sarah</creator><creator>Bryan, Nick D.</creator><creator>Keith-Roach, Miranda J.</creator><general>Elsevier Ltd</general><general>Elsevier</general><scope>FBQ</scope><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>7X8</scope></search><sort><creationdate>20121001</creationdate><title>The effect of EDTA on the groundwater transport of thorium through sand</title><author>May, Colin C. ; Young, Lindsay ; Worsfold, Paul J. ; Heath, Sarah ; Bryan, Nick D. ; Keith-Roach, Miranda J.</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c416t-d59fbbd78a61465a4430db207c28c3f1f35fc602fedf3c2d65d2e440dcd9d5ba3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2012</creationdate><topic>Applied sciences</topic><topic>Colloid</topic><topic>colloids</topic><topic>Complexation</topic><topic>Complexing agent</topic><topic>Edetic Acid - chemistry</topic><topic>EDTA (chelating agent)</topic><topic>Exact sciences and technology</topic><topic>Groundwater - chemistry</topic><topic>groundwater flow</topic><topic>Migration</topic><topic>Modelling</topic><topic>Models, Theoretical</topic><topic>Pollution</topic><topic>sand</topic><topic>Silicon Dioxide</topic><topic>Speciation</topic><topic>thorium</topic><topic>Thorium - chemistry</topic><topic>uncertainty</topic><topic>Water treatment and pollution</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>May, Colin C.</creatorcontrib><creatorcontrib>Young, Lindsay</creatorcontrib><creatorcontrib>Worsfold, Paul J.</creatorcontrib><creatorcontrib>Heath, Sarah</creatorcontrib><creatorcontrib>Bryan, Nick D.</creatorcontrib><creatorcontrib>Keith-Roach, Miranda J.</creatorcontrib><collection>AGRIS</collection><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>MEDLINE - Academic</collection><jtitle>Water research (Oxford)</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>May, Colin C.</au><au>Young, Lindsay</au><au>Worsfold, Paul J.</au><au>Heath, Sarah</au><au>Bryan, Nick D.</au><au>Keith-Roach, Miranda J.</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>The effect of EDTA on the groundwater transport of thorium through sand</atitle><jtitle>Water research (Oxford)</jtitle><addtitle>Water Res</addtitle><date>2012-10-01</date><risdate>2012</risdate><volume>46</volume><issue>15</issue><spage>4870</spage><epage>4882</epage><pages>4870-4882</pages><issn>0043-1354</issn><eissn>1879-2448</eissn><coden>WATRAG</coden><abstract>The effect of the anthropogenic complexing agent EDTA on thorium transport in groundwater has been studied using sand-packed columns and flow rates in the range of 20–100 m y−1. The concentrations injected into the columns were in the range of 0.4–4 mM for Th and 4–40 mM for EDTA, and with EDTA:Th ratios in the range 1:1 to 10:1. The results show that EDTA can significantly increase Th transport, but two very different behaviours are observed at Th concentrations of 0.4 and 4 mM. At the lower concentration, Th breakthrough is retarded with respect to a conservative tracer, with a peak width that is consistent with a single Kd value, followed by a longer tail, and the behaviour is very sensitive to the flow rate. However at 4 mM Th, the breakthrough peak appears near to that of the tracer, and the width of the peak is consistent with a distribution of Kd values and/or a larger dispersivity than the tracer. Speciation and transport modelling have been used to interpret the data, and a model was developed that could explain the 0.4 mM behaviour. This suggests that ternary surface complexes are important in these systems, with at least two different species involved, although the complexity of Th speciation in these systems leads to significant uncertainty in the values of the equilibrium and kinetic parameters. For the 4 mM systems, the rapid transport observed could not be explained by a simple chemical model; instead it is likely that EDTA plays an important role in stabilising and transporting thorium colloids and clusters. [Display omitted] ► EDTA has been shown to enhance thorium migration through sand significantly. ► Transport involves ternary interactions between Th-EDTA complexes and the sand. ► The concentration of thorium and EDTA affects the transport mechanism. ► A simple chemical model has been developed to explain thorium behaviour at low concentrations. ► Evidence is provided for mobile EDTA-stabilised thorium colloidal transport at high thorium and EDTA concentrations.</abstract><cop>Kidlington</cop><pub>Elsevier Ltd</pub><pmid>22796006</pmid><doi>10.1016/j.watres.2012.06.012</doi><tpages>13</tpages></addata></record>
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source MEDLINE; Elsevier ScienceDirect Journals
subjects Applied sciences
Colloid
colloids
Complexation
Complexing agent
Edetic Acid - chemistry
EDTA (chelating agent)
Exact sciences and technology
Groundwater - chemistry
groundwater flow
Migration
Modelling
Models, Theoretical
Pollution
sand
Silicon Dioxide
Speciation
thorium
Thorium - chemistry
uncertainty
Water treatment and pollution
title The effect of EDTA on the groundwater transport of thorium through sand
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