The role of thermal and photochemical reactions upon the remobilisation of Pu from an Irish Sea sediment
Laboratory experiments were carried out to assess the influence of temperature and photochemical reactions upon the dissolution of 239+240Pu and 241Am from an Irish Sea sediment in seawater. Supplementary information was obtained from experiments to evaluate the rate and extent of 239Np tracer desor...
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Veröffentlicht in: | Journal of environmental radioactivity 1999-01, Vol.44 (2), p.253-273 |
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container_title | Journal of environmental radioactivity |
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creator | McCubbin, David Leonard, Kinson S. Emerson, Heather S. |
description | Laboratory experiments were carried out to assess the influence of temperature and photochemical reactions upon the dissolution of
239+240Pu and
241Am from an Irish Sea sediment in seawater. Supplementary information was obtained from experiments to evaluate the rate and extent of
239Np tracer desorption, and
238Pu(V) tracer uptake. A steady state distribution of
241Am and
239+240Pu(IV) species between dissolved and particulate phases was rapidly attained ( |
doi_str_mv | 10.1016/S0265-931X(98)00136-2 |
format | Article |
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239+240Pu and
241Am from an Irish Sea sediment in seawater. Supplementary information was obtained from experiments to evaluate the rate and extent of
239Np tracer desorption, and
238Pu(V) tracer uptake. A steady state distribution of
241Am and
239+240Pu(IV) species between dissolved and particulate phases was rapidly attained (<1 h). The extent of their remobilisation was largely unaffected by temperature changes within the range ≈4–25°C and light irradiation. Dissolution of Pu(V) species appeared to occur as an independent process and the data could be modelled in terms of a reversible first order reaction. Remobilisation of
239+240Pu(V), and uptake of
238Pu(V) tracer, species increased concomitant with temperature and light irradiation due to simultaneous promotion of oxidation and reduction reactions upon the surface of the suspended particles. It is suggested that, in terms of band-gap theory, the rate determining step may be migration of valence band holes and conduction electrons to Pu sites. These laboratory data are discussed in the context of extrapolating trends to the remobilisation behaviour of
239+240Pu and
241Am from contaminated sediments in the Irish Sea (UK). An assessment is made of the half-time taken for Pu(V) species to attain a steady-state distribution between dissolved and particulate phases. These estimates are compared with the predicted half-time for dissolution of
239+240Pu bound to Irish Sea sediments.</description><identifier>ISSN: 0265-931X</identifier><identifier>EISSN: 1879-1700</identifier><identifier>DOI: 10.1016/S0265-931X(98)00136-2</identifier><language>eng</language><publisher>Elsevier Ltd</publisher><subject>Photochemistry ; Plutonium ; Remobilisation ; Seawater ; Sorption ; Temperature</subject><ispartof>Journal of environmental radioactivity, 1999-01, Vol.44 (2), p.253-273</ispartof><rights>1999</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c338t-144187095ab2cd0f1058cc1bfb27e007ee4f25de9f386191796802d71e6b0cb23</citedby></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktohtml>$$Uhttps://www.sciencedirect.com/science/article/pii/S0265931X98001362$$EHTML$$P50$$Gelsevier$$H</linktohtml><link.rule.ids>314,776,780,3537,27901,27902,65306</link.rule.ids></links><search><creatorcontrib>McCubbin, David</creatorcontrib><creatorcontrib>Leonard, Kinson S.</creatorcontrib><creatorcontrib>Emerson, Heather S.</creatorcontrib><title>The role of thermal and photochemical reactions upon the remobilisation of Pu from an Irish Sea sediment</title><title>Journal of environmental radioactivity</title><description>Laboratory experiments were carried out to assess the influence of temperature and photochemical reactions upon the dissolution of
239+240Pu and
241Am from an Irish Sea sediment in seawater. Supplementary information was obtained from experiments to evaluate the rate and extent of
239Np tracer desorption, and
238Pu(V) tracer uptake. A steady state distribution of
241Am and
239+240Pu(IV) species between dissolved and particulate phases was rapidly attained (<1 h). The extent of their remobilisation was largely unaffected by temperature changes within the range ≈4–25°C and light irradiation. Dissolution of Pu(V) species appeared to occur as an independent process and the data could be modelled in terms of a reversible first order reaction. Remobilisation of
239+240Pu(V), and uptake of
238Pu(V) tracer, species increased concomitant with temperature and light irradiation due to simultaneous promotion of oxidation and reduction reactions upon the surface of the suspended particles. It is suggested that, in terms of band-gap theory, the rate determining step may be migration of valence band holes and conduction electrons to Pu sites. These laboratory data are discussed in the context of extrapolating trends to the remobilisation behaviour of
239+240Pu and
241Am from contaminated sediments in the Irish Sea (UK). An assessment is made of the half-time taken for Pu(V) species to attain a steady-state distribution between dissolved and particulate phases. These estimates are compared with the predicted half-time for dissolution of
239+240Pu bound to Irish Sea sediments.</description><subject>Photochemistry</subject><subject>Plutonium</subject><subject>Remobilisation</subject><subject>Seawater</subject><subject>Sorption</subject><subject>Temperature</subject><issn>0265-931X</issn><issn>1879-1700</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>1999</creationdate><recordtype>article</recordtype><recordid>eNqFkE9LxDAQxYMouK5-BCEn0UN1km7b5CSy-GdhQWFX8BbSdEIjbbMmreC3t3XFq6eBN783zHuEnDO4ZsDymw3wPEtkyt4upbgCYGme8AMyY6KQCSsADsnsDzkmJzG-j1ABgs9Iva2RBt8g9Zb2NYZWN1R3Fd3VvvemxtaZUQmoTe98F-mw890EjlLrS9e4qKfFZH8ZqA2-He10FVys6QY1jVi5Frv-lBxZ3UQ8-51z8vpwv10-Jevnx9Xybp2YNBV9whaL8W2QmS65qcAyyIQxrLQlLxCgQFxYnlUobSpyJlkhcwG8KhjmJZiSp3Nysb-7C_5jwNir1kWDTaM79ENUrOAi42ICsz1ogo8xoFW74FodvhQDNfWqfnpVU2lKCvXTq5p8t3sfjik-HQYVjcPOjDkDml5V3v1z4RvcgYCH</recordid><startdate>19990101</startdate><enddate>19990101</enddate><creator>McCubbin, David</creator><creator>Leonard, Kinson S.</creator><creator>Emerson, Heather S.</creator><general>Elsevier Ltd</general><scope>AAYXX</scope><scope>CITATION</scope><scope>7TV</scope><scope>7UA</scope><scope>C1K</scope><scope>F1W</scope><scope>H97</scope><scope>L.G</scope></search><sort><creationdate>19990101</creationdate><title>The role of thermal and photochemical reactions upon the remobilisation of Pu from an Irish Sea sediment</title><author>McCubbin, David ; Leonard, Kinson S. ; Emerson, Heather S.</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c338t-144187095ab2cd0f1058cc1bfb27e007ee4f25de9f386191796802d71e6b0cb23</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>1999</creationdate><topic>Photochemistry</topic><topic>Plutonium</topic><topic>Remobilisation</topic><topic>Seawater</topic><topic>Sorption</topic><topic>Temperature</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>McCubbin, David</creatorcontrib><creatorcontrib>Leonard, Kinson S.</creatorcontrib><creatorcontrib>Emerson, Heather S.</creatorcontrib><collection>CrossRef</collection><collection>Pollution Abstracts</collection><collection>Water Resources Abstracts</collection><collection>Environmental Sciences and Pollution Management</collection><collection>ASFA: Aquatic Sciences and Fisheries Abstracts</collection><collection>Aquatic Science & Fisheries Abstracts (ASFA) 3: Aquatic Pollution & Environmental Quality</collection><collection>Aquatic Science & Fisheries Abstracts (ASFA) Professional</collection><jtitle>Journal of environmental radioactivity</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>McCubbin, David</au><au>Leonard, Kinson S.</au><au>Emerson, Heather S.</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>The role of thermal and photochemical reactions upon the remobilisation of Pu from an Irish Sea sediment</atitle><jtitle>Journal of environmental radioactivity</jtitle><date>1999-01-01</date><risdate>1999</risdate><volume>44</volume><issue>2</issue><spage>253</spage><epage>273</epage><pages>253-273</pages><issn>0265-931X</issn><eissn>1879-1700</eissn><abstract>Laboratory experiments were carried out to assess the influence of temperature and photochemical reactions upon the dissolution of
239+240Pu and
241Am from an Irish Sea sediment in seawater. Supplementary information was obtained from experiments to evaluate the rate and extent of
239Np tracer desorption, and
238Pu(V) tracer uptake. A steady state distribution of
241Am and
239+240Pu(IV) species between dissolved and particulate phases was rapidly attained (<1 h). The extent of their remobilisation was largely unaffected by temperature changes within the range ≈4–25°C and light irradiation. Dissolution of Pu(V) species appeared to occur as an independent process and the data could be modelled in terms of a reversible first order reaction. Remobilisation of
239+240Pu(V), and uptake of
238Pu(V) tracer, species increased concomitant with temperature and light irradiation due to simultaneous promotion of oxidation and reduction reactions upon the surface of the suspended particles. It is suggested that, in terms of band-gap theory, the rate determining step may be migration of valence band holes and conduction electrons to Pu sites. These laboratory data are discussed in the context of extrapolating trends to the remobilisation behaviour of
239+240Pu and
241Am from contaminated sediments in the Irish Sea (UK). An assessment is made of the half-time taken for Pu(V) species to attain a steady-state distribution between dissolved and particulate phases. These estimates are compared with the predicted half-time for dissolution of
239+240Pu bound to Irish Sea sediments.</abstract><pub>Elsevier Ltd</pub><doi>10.1016/S0265-931X(98)00136-2</doi><tpages>21</tpages></addata></record> |
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ispartof | Journal of environmental radioactivity, 1999-01, Vol.44 (2), p.253-273 |
issn | 0265-931X 1879-1700 |
language | eng |
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source | Elsevier ScienceDirect Journals |
subjects | Photochemistry Plutonium Remobilisation Seawater Sorption Temperature |
title | The role of thermal and photochemical reactions upon the remobilisation of Pu from an Irish Sea sediment |
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