Actinide Lanthanide Separation ProcessALSEP
Separation of the minor actinides (Am, Cm) from the lanthanides at an industrial scale remains a significant technical challenge for closing the nuclear fuel cycle. To increase the safety of used nuclear fuel (UNF) reprocessing, as well as reduce associated costs, a novel solvent extraction process...
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Veröffentlicht in: | Industrial & engineering chemistry research 2014-01, Vol.53 (4), p.1624-1631 |
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description | Separation of the minor actinides (Am, Cm) from the lanthanides at an industrial scale remains a significant technical challenge for closing the nuclear fuel cycle. To increase the safety of used nuclear fuel (UNF) reprocessing, as well as reduce associated costs, a novel solvent extraction process has been developed. The process allows for partitioning minor actinides, lanthanides, and fission products following uranium/plutonium/neptunium removal, minimizing the number of separation steps, flowsheets, chemical consumption, and waste. This new process, actinide lanthanide separation (ALSEP), uses an organic solvent consisting of a neutral diglycolamide extractant, either N,N,N′,N′-tetra(2-ethylhexyl)diglycolamide (T2EHDGA) or N,N,N′,N′-tetraoctyldiglycolamide (TODGA), and an acidic extractant 2-ethylhexylphosphonic acid mono-2-ethylhexyl ester (HEH[EHP]), dissolved in an aliphatic diluent (e.g., n-dodecane). The An/Ln coextraction is conducted from moderate-to-strong nitric acid, while the selective stripping of the minor actinides from the lanthanides is carried out using a polyaminocarboxylic acid/citrate buffered solution at pH anywhere between 3 and 4.5. The extraction and separation of the actinides from the fission products is very effective in a wide range of HNO3 concentrations, and the minimum separation factors for lanthanide/Am exceed 30 for Nd/Am, reaching >60 for Eu/Am under some conditions. The experimental results presented here demonstrate the great potential for a combined system, consisting of a neutral extractant such as T2EHDGA or TODGA, and an acidic extractant such as HEH[EHP], for separating the minor actinides from the lanthanides. |
doi_str_mv | 10.1021/ie403569e |
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(PNNL), Richland, WA (United States)</creatorcontrib><description>Separation of the minor actinides (Am, Cm) from the lanthanides at an industrial scale remains a significant technical challenge for closing the nuclear fuel cycle. To increase the safety of used nuclear fuel (UNF) reprocessing, as well as reduce associated costs, a novel solvent extraction process has been developed. The process allows for partitioning minor actinides, lanthanides, and fission products following uranium/plutonium/neptunium removal, minimizing the number of separation steps, flowsheets, chemical consumption, and waste. This new process, actinide lanthanide separation (ALSEP), uses an organic solvent consisting of a neutral diglycolamide extractant, either N,N,N′,N′-tetra(2-ethylhexyl)diglycolamide (T2EHDGA) or N,N,N′,N′-tetraoctyldiglycolamide (TODGA), and an acidic extractant 2-ethylhexylphosphonic acid mono-2-ethylhexyl ester (HEH[EHP]), dissolved in an aliphatic diluent (e.g., n-dodecane). The An/Ln coextraction is conducted from moderate-to-strong nitric acid, while the selective stripping of the minor actinides from the lanthanides is carried out using a polyaminocarboxylic acid/citrate buffered solution at pH anywhere between 3 and 4.5. The extraction and separation of the actinides from the fission products is very effective in a wide range of HNO3 concentrations, and the minimum separation factors for lanthanide/Am exceed 30 for Nd/Am, reaching >60 for Eu/Am under some conditions. The experimental results presented here demonstrate the great potential for a combined system, consisting of a neutral extractant such as T2EHDGA or TODGA, and an acidic extractant such as HEH[EHP], for separating the minor actinides from the lanthanides.</description><identifier>ISSN: 0888-5885</identifier><identifier>EISSN: 1520-5045</identifier><identifier>DOI: 10.1021/ie403569e</identifier><language>eng</language><publisher>United States: American Chemical Society</publisher><subject>actinide separation ; Actinides ; ALSEP ; Fission products ; HEH[EHP] ; lanthanide separation ; Lanthanides ; Nuclear fuels ; Partitioning ; Plutonium ; Separation ; Solvent extraction ; T2EHDGA ; TODGA</subject><ispartof>Industrial & engineering chemistry research, 2014-01, Vol.53 (4), p.1624-1631</ispartof><rights>Copyright © 2014 American Chemical Society</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-a356t-492b091c4cc0bf5565bf9dca8fb48fcdb329c65435210dfad8fdd3a778a3bd2f3</citedby><cites>FETCH-LOGICAL-a356t-492b091c4cc0bf5565bf9dca8fb48fcdb329c65435210dfad8fdd3a778a3bd2f3</cites></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://pubs.acs.org/doi/pdf/10.1021/ie403569e$$EPDF$$P50$$Gacs$$H</linktopdf><linktohtml>$$Uhttps://pubs.acs.org/doi/10.1021/ie403569e$$EHTML$$P50$$Gacs$$H</linktohtml><link.rule.ids>314,776,780,881,2752,27053,27901,27902,56713,56763</link.rule.ids><backlink>$$Uhttps://www.osti.gov/biblio/1130192$$D View this record in Osti.gov$$Hfree_for_read</backlink></links><search><creatorcontrib>Gelis, Artem V</creatorcontrib><creatorcontrib>Lumetta, Gregg J</creatorcontrib><creatorcontrib>Pacific Northwest National Lab. (PNNL), Richland, WA (United States)</creatorcontrib><title>Actinide Lanthanide Separation ProcessALSEP</title><title>Industrial & engineering chemistry research</title><addtitle>Ind. Eng. Chem. Res</addtitle><description>Separation of the minor actinides (Am, Cm) from the lanthanides at an industrial scale remains a significant technical challenge for closing the nuclear fuel cycle. To increase the safety of used nuclear fuel (UNF) reprocessing, as well as reduce associated costs, a novel solvent extraction process has been developed. The process allows for partitioning minor actinides, lanthanides, and fission products following uranium/plutonium/neptunium removal, minimizing the number of separation steps, flowsheets, chemical consumption, and waste. This new process, actinide lanthanide separation (ALSEP), uses an organic solvent consisting of a neutral diglycolamide extractant, either N,N,N′,N′-tetra(2-ethylhexyl)diglycolamide (T2EHDGA) or N,N,N′,N′-tetraoctyldiglycolamide (TODGA), and an acidic extractant 2-ethylhexylphosphonic acid mono-2-ethylhexyl ester (HEH[EHP]), dissolved in an aliphatic diluent (e.g., n-dodecane). The An/Ln coextraction is conducted from moderate-to-strong nitric acid, while the selective stripping of the minor actinides from the lanthanides is carried out using a polyaminocarboxylic acid/citrate buffered solution at pH anywhere between 3 and 4.5. The extraction and separation of the actinides from the fission products is very effective in a wide range of HNO3 concentrations, and the minimum separation factors for lanthanide/Am exceed 30 for Nd/Am, reaching >60 for Eu/Am under some conditions. The experimental results presented here demonstrate the great potential for a combined system, consisting of a neutral extractant such as T2EHDGA or TODGA, and an acidic extractant such as HEH[EHP], for separating the minor actinides from the lanthanides.</description><subject>actinide separation</subject><subject>Actinides</subject><subject>ALSEP</subject><subject>Fission products</subject><subject>HEH[EHP]</subject><subject>lanthanide separation</subject><subject>Lanthanides</subject><subject>Nuclear fuels</subject><subject>Partitioning</subject><subject>Plutonium</subject><subject>Separation</subject><subject>Solvent extraction</subject><subject>T2EHDGA</subject><subject>TODGA</subject><issn>0888-5885</issn><issn>1520-5045</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2014</creationdate><recordtype>article</recordtype><recordid>eNpt0M9KAzEQBvAgCtbqwTcogqCHrckm2WaPpdQ_sGCheg7ZSUJT2qQm6cEn8VX6VD6DqyuePM0cfnzDfAhdEjwmuCR3zjBMeVWbIzQgvMQFx4wfowEWQhRcCH6KzlJaY4w5Z2yAxlPIzjttRo3yeaV-1qXZqaiyC360iAFMSp8fh2mznC_O0YlVm2QufucQvd7PX2aPRfP88DSbNoXqjueC1WWLawIMALeW84q3ttaghG2ZsKBbWtZQcUZ5SbC2SgurNVWTiVC01aWlQ3TV54aUnUzgsoEVBO8NZEkIxaQuO3TTo10Mb3uTsty6BGazUd6EfZKk6hBlhFQdve0pxJBSNFbuotuq-C4Jlt_Fyb_iOnvdWwVJrsM--u7Tf9wXsO9sJQ</recordid><startdate>20140129</startdate><enddate>20140129</enddate><creator>Gelis, Artem V</creator><creator>Lumetta, Gregg J</creator><general>American Chemical Society</general><scope>AAYXX</scope><scope>CITATION</scope><scope>7SR</scope><scope>8BQ</scope><scope>8FD</scope><scope>JG9</scope><scope>OTOTI</scope></search><sort><creationdate>20140129</creationdate><title>Actinide Lanthanide Separation ProcessALSEP</title><author>Gelis, Artem V ; Lumetta, Gregg J</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-a356t-492b091c4cc0bf5565bf9dca8fb48fcdb329c65435210dfad8fdd3a778a3bd2f3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2014</creationdate><topic>actinide separation</topic><topic>Actinides</topic><topic>ALSEP</topic><topic>Fission products</topic><topic>HEH[EHP]</topic><topic>lanthanide separation</topic><topic>Lanthanides</topic><topic>Nuclear fuels</topic><topic>Partitioning</topic><topic>Plutonium</topic><topic>Separation</topic><topic>Solvent extraction</topic><topic>T2EHDGA</topic><topic>TODGA</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Gelis, Artem V</creatorcontrib><creatorcontrib>Lumetta, Gregg J</creatorcontrib><creatorcontrib>Pacific Northwest National Lab. (PNNL), Richland, WA (United States)</creatorcontrib><collection>CrossRef</collection><collection>Engineered Materials Abstracts</collection><collection>METADEX</collection><collection>Technology Research Database</collection><collection>Materials Research Database</collection><collection>OSTI.GOV</collection><jtitle>Industrial & engineering chemistry research</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Gelis, Artem V</au><au>Lumetta, Gregg J</au><aucorp>Pacific Northwest National Lab. (PNNL), Richland, WA (United States)</aucorp><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Actinide Lanthanide Separation ProcessALSEP</atitle><jtitle>Industrial & engineering chemistry research</jtitle><addtitle>Ind. Eng. Chem. Res</addtitle><date>2014-01-29</date><risdate>2014</risdate><volume>53</volume><issue>4</issue><spage>1624</spage><epage>1631</epage><pages>1624-1631</pages><issn>0888-5885</issn><eissn>1520-5045</eissn><abstract>Separation of the minor actinides (Am, Cm) from the lanthanides at an industrial scale remains a significant technical challenge for closing the nuclear fuel cycle. To increase the safety of used nuclear fuel (UNF) reprocessing, as well as reduce associated costs, a novel solvent extraction process has been developed. The process allows for partitioning minor actinides, lanthanides, and fission products following uranium/plutonium/neptunium removal, minimizing the number of separation steps, flowsheets, chemical consumption, and waste. This new process, actinide lanthanide separation (ALSEP), uses an organic solvent consisting of a neutral diglycolamide extractant, either N,N,N′,N′-tetra(2-ethylhexyl)diglycolamide (T2EHDGA) or N,N,N′,N′-tetraoctyldiglycolamide (TODGA), and an acidic extractant 2-ethylhexylphosphonic acid mono-2-ethylhexyl ester (HEH[EHP]), dissolved in an aliphatic diluent (e.g., n-dodecane). The An/Ln coextraction is conducted from moderate-to-strong nitric acid, while the selective stripping of the minor actinides from the lanthanides is carried out using a polyaminocarboxylic acid/citrate buffered solution at pH anywhere between 3 and 4.5. The extraction and separation of the actinides from the fission products is very effective in a wide range of HNO3 concentrations, and the minimum separation factors for lanthanide/Am exceed 30 for Nd/Am, reaching >60 for Eu/Am under some conditions. The experimental results presented here demonstrate the great potential for a combined system, consisting of a neutral extractant such as T2EHDGA or TODGA, and an acidic extractant such as HEH[EHP], for separating the minor actinides from the lanthanides.</abstract><cop>United States</cop><pub>American Chemical Society</pub><doi>10.1021/ie403569e</doi><tpages>8</tpages></addata></record> |
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subjects | actinide separation Actinides ALSEP Fission products HEH[EHP] lanthanide separation Lanthanides Nuclear fuels Partitioning Plutonium Separation Solvent extraction T2EHDGA TODGA |
title | Actinide Lanthanide Separation ProcessALSEP |
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