Thermodynamic Model for Uranium Release from Hanford Site Tank Residual Waste
A thermodynamic model of U solid-phase solubility and paragenesis was developed for Hanford Site tank residual waste that will remain in place after tank closure. The model was developed using a combination of waste composition data, waste leach test data, and thermodynamic modeling of the leach tes...
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| Veröffentlicht in: | Environmental science & technology 2011-02, Vol.45 (4), p.1473-1480 |
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| creator | Cantrell, Kirk J Deutsch, William J Lindberg, Mike J |
| description | A thermodynamic model of U solid-phase solubility and paragenesis was developed for Hanford Site tank residual waste that will remain in place after tank closure. The model was developed using a combination of waste composition data, waste leach test data, and thermodynamic modeling of the leach test data. The testing and analyses were conducted using actual Hanford Site tank residual waste. Positive identification of U phases by X-ray diffraction was generally not possible either because solids in the waste were amorphous or their concentrations were not detectable by XRD for both as-received and leached residual waste. Three leachant solutions were used in the studies: deionized water, CaCO3 saturated solution, and Ca(OH)2 saturated solution. Analysis of calculated saturation indices indicate that NaUO2PO4·xH2O and Na2U2O7(am) are present in the residual wastes initially. Leaching of the residual wastes with deionized water or CaCO3 saturated solution results in preferential dissolution Na2U2O7(am) and formation of schoepite. Leaching of the residual wastes with Ca(OH)2 saturated solution appears to result in transformation of both NaUO2PO4·xH2O and Na2U2O7(am) to CaUO4. Upon the basis of these results, the paragenetic sequence of secondary phases expected to occur as leaching of residual waste progresses for two tank closure scenarios was identified. |
| doi_str_mv | 10.1021/es1038968 |
| format | Article |
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(PNNL), Richland, WA (United States)</creatorcontrib><description>A thermodynamic model of U solid-phase solubility and paragenesis was developed for Hanford Site tank residual waste that will remain in place after tank closure. The model was developed using a combination of waste composition data, waste leach test data, and thermodynamic modeling of the leach test data. The testing and analyses were conducted using actual Hanford Site tank residual waste. Positive identification of U phases by X-ray diffraction was generally not possible either because solids in the waste were amorphous or their concentrations were not detectable by XRD for both as-received and leached residual waste. Three leachant solutions were used in the studies: deionized water, CaCO3 saturated solution, and Ca(OH)2 saturated solution. Analysis of calculated saturation indices indicate that NaUO2PO4·xH2O and Na2U2O7(am) are present in the residual wastes initially. Leaching of the residual wastes with deionized water or CaCO3 saturated solution results in preferential dissolution Na2U2O7(am) and formation of schoepite. Leaching of the residual wastes with Ca(OH)2 saturated solution appears to result in transformation of both NaUO2PO4·xH2O and Na2U2O7(am) to CaUO4. Upon the basis of these results, the paragenetic sequence of secondary phases expected to occur as leaching of residual waste progresses for two tank closure scenarios was identified.</description><identifier>ISSN: 0013-936X</identifier><identifier>EISSN: 1520-5851</identifier><identifier>DOI: 10.1021/es1038968</identifier><identifier>PMID: 21268633</identifier><identifier>CODEN: ESTHAG</identifier><language>eng</language><publisher>Washington, DC: American Chemical Society</publisher><subject>Applied sciences ; CLOSURES ; DESIGN ; Earth sciences ; Earth, ocean, space ; Engineering and environment geology. Geothermics ; Environmental Modeling ; Environmental science ; ENVIRONMENTAL SCIENCES ; Exact sciences and technology ; Hanford tank residual waste ; LEACHING ; Models, Theoretical ; Pollution ; Pollution, environment geology ; Radioactive Waste - analysis ; Radioactive wastes ; SENSITIVITY ; SIMULATION ; single-shell tanks ; SOLUBILITY ; TANKS ; TESTING ; THERMODYNAMIC MODEL ; THERMODYNAMICS ; U solubility ; URANIUM ; Uranium - analysis ; Waste materials ; WASTES ; WATER ; X-RAY DIFFRACTION</subject><ispartof>Environmental science & technology, 2011-02, Vol.45 (4), p.1473-1480</ispartof><rights>Copyright © 2011 American Chemical Society</rights><rights>2015 INIST-CNRS</rights><rights>Copyright American Chemical Society Feb 15, 2011</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-a399t-d813c0e89fc569498a33c690f652dda819ff268f938e21325937c06665e266ab3</citedby><cites>FETCH-LOGICAL-a399t-d813c0e89fc569498a33c690f652dda819ff268f938e21325937c06665e266ab3</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/es1038968$$EPDF$$P50$$Gacs$$H</linktopdf><linktohtml>$$Uhttps://pubs.acs.org/doi/10.1021/es1038968$$EHTML$$P50$$Gacs$$H</linktohtml><link.rule.ids>230,314,776,780,881,2752,27053,27901,27902,56713,56763</link.rule.ids><backlink>$$Uhttp://pascal-francis.inist.fr/vibad/index.php?action=getRecordDetail&idt=24167019$$DView record in Pascal Francis$$Hfree_for_read</backlink><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/21268633$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink><backlink>$$Uhttps://www.osti.gov/biblio/1007349$$D View this record in Osti.gov$$Hfree_for_read</backlink></links><search><creatorcontrib>Cantrell, Kirk J</creatorcontrib><creatorcontrib>Deutsch, William J</creatorcontrib><creatorcontrib>Lindberg, Mike J</creatorcontrib><creatorcontrib>Pacific Northwest National Lab. (PNNL), Richland, WA (United States)</creatorcontrib><title>Thermodynamic Model for Uranium Release from Hanford Site Tank Residual Waste</title><title>Environmental science & technology</title><addtitle>Environ. Sci. Technol</addtitle><description>A thermodynamic model of U solid-phase solubility and paragenesis was developed for Hanford Site tank residual waste that will remain in place after tank closure. The model was developed using a combination of waste composition data, waste leach test data, and thermodynamic modeling of the leach test data. The testing and analyses were conducted using actual Hanford Site tank residual waste. Positive identification of U phases by X-ray diffraction was generally not possible either because solids in the waste were amorphous or their concentrations were not detectable by XRD for both as-received and leached residual waste. Three leachant solutions were used in the studies: deionized water, CaCO3 saturated solution, and Ca(OH)2 saturated solution. Analysis of calculated saturation indices indicate that NaUO2PO4·xH2O and Na2U2O7(am) are present in the residual wastes initially. Leaching of the residual wastes with deionized water or CaCO3 saturated solution results in preferential dissolution Na2U2O7(am) and formation of schoepite. Leaching of the residual wastes with Ca(OH)2 saturated solution appears to result in transformation of both NaUO2PO4·xH2O and Na2U2O7(am) to CaUO4. Upon the basis of these results, the paragenetic sequence of secondary phases expected to occur as leaching of residual waste progresses for two tank closure scenarios was identified.</description><subject>Applied sciences</subject><subject>CLOSURES</subject><subject>DESIGN</subject><subject>Earth sciences</subject><subject>Earth, ocean, space</subject><subject>Engineering and environment geology. Geothermics</subject><subject>Environmental Modeling</subject><subject>Environmental science</subject><subject>ENVIRONMENTAL SCIENCES</subject><subject>Exact sciences and technology</subject><subject>Hanford tank residual waste</subject><subject>LEACHING</subject><subject>Models, Theoretical</subject><subject>Pollution</subject><subject>Pollution, environment geology</subject><subject>Radioactive Waste - analysis</subject><subject>Radioactive wastes</subject><subject>SENSITIVITY</subject><subject>SIMULATION</subject><subject>single-shell tanks</subject><subject>SOLUBILITY</subject><subject>TANKS</subject><subject>TESTING</subject><subject>THERMODYNAMIC MODEL</subject><subject>THERMODYNAMICS</subject><subject>U solubility</subject><subject>URANIUM</subject><subject>Uranium - analysis</subject><subject>Waste materials</subject><subject>WASTES</subject><subject>WATER</subject><subject>X-RAY DIFFRACTION</subject><issn>0013-936X</issn><issn>1520-5851</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2011</creationdate><recordtype>article</recordtype><sourceid>EIF</sourceid><recordid>eNpl0cFu1DAQBmALUdGlcOAFkIWEBIeA7Um89hFVQJFaVYKt4BZNnbGaksStJzn07Wu0y-6hJx_m0z_jGSHeaPVJK6M_E2sFzlv3TKx0Y1TVuEY_FyulNFQe7J9j8ZL5VillQLkX4thoY50FWImLzQ3lMXUPE459kBepo0HGlOVVxqlfRvmTBkImGXMa5RlOpdbJX_1McoPT31LmvltwkL-RZ3oljiIOTK9374m4-vZ1c3pWnV9-_3H65bxC8H6uOqchKHI-hsb62jsECNaraBvTdei0j7EMGD04MhpM42EdlLW2IWMtXsOJeLfNTTz3LYcyTrgJaZoozK1Wag21L-jDFt3ldL8Qz-3Yc6BhwInSwm0JBrMuW3OHvD29TUueyhda19Q1WAO2oI9bFHJizhTbu9yPmB9Kx_bfHdr9HYp9uwtcrkfq9vL_4gt4vwPIAYdYth16Prha27XS_uAw8GGopw0fASqIl_A</recordid><startdate>20110215</startdate><enddate>20110215</enddate><creator>Cantrell, Kirk J</creator><creator>Deutsch, William J</creator><creator>Lindberg, Mike J</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>20110215</creationdate><title>Thermodynamic Model for Uranium Release from Hanford Site Tank Residual Waste</title><author>Cantrell, Kirk J ; Deutsch, William J ; Lindberg, Mike J</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-a399t-d813c0e89fc569498a33c690f652dda819ff268f938e21325937c06665e266ab3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2011</creationdate><topic>Applied sciences</topic><topic>CLOSURES</topic><topic>DESIGN</topic><topic>Earth sciences</topic><topic>Earth, ocean, space</topic><topic>Engineering and environment geology. Geothermics</topic><topic>Environmental Modeling</topic><topic>Environmental science</topic><topic>ENVIRONMENTAL SCIENCES</topic><topic>Exact sciences and technology</topic><topic>Hanford tank residual waste</topic><topic>LEACHING</topic><topic>Models, Theoretical</topic><topic>Pollution</topic><topic>Pollution, environment geology</topic><topic>Radioactive Waste - analysis</topic><topic>Radioactive wastes</topic><topic>SENSITIVITY</topic><topic>SIMULATION</topic><topic>single-shell tanks</topic><topic>SOLUBILITY</topic><topic>TANKS</topic><topic>TESTING</topic><topic>THERMODYNAMIC MODEL</topic><topic>THERMODYNAMICS</topic><topic>U solubility</topic><topic>URANIUM</topic><topic>Uranium - analysis</topic><topic>Waste materials</topic><topic>WASTES</topic><topic>WATER</topic><topic>X-RAY DIFFRACTION</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Cantrell, Kirk J</creatorcontrib><creatorcontrib>Deutsch, William J</creatorcontrib><creatorcontrib>Lindberg, Mike J</creatorcontrib><creatorcontrib>Pacific Northwest National Lab. 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(PNNL), Richland, WA (United States)</aucorp><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Thermodynamic Model for Uranium Release from Hanford Site Tank Residual Waste</atitle><jtitle>Environmental science & technology</jtitle><addtitle>Environ. Sci. Technol</addtitle><date>2011-02-15</date><risdate>2011</risdate><volume>45</volume><issue>4</issue><spage>1473</spage><epage>1480</epage><pages>1473-1480</pages><issn>0013-936X</issn><eissn>1520-5851</eissn><coden>ESTHAG</coden><abstract>A thermodynamic model of U solid-phase solubility and paragenesis was developed for Hanford Site tank residual waste that will remain in place after tank closure. The model was developed using a combination of waste composition data, waste leach test data, and thermodynamic modeling of the leach test data. The testing and analyses were conducted using actual Hanford Site tank residual waste. Positive identification of U phases by X-ray diffraction was generally not possible either because solids in the waste were amorphous or their concentrations were not detectable by XRD for both as-received and leached residual waste. Three leachant solutions were used in the studies: deionized water, CaCO3 saturated solution, and Ca(OH)2 saturated solution. Analysis of calculated saturation indices indicate that NaUO2PO4·xH2O and Na2U2O7(am) are present in the residual wastes initially. Leaching of the residual wastes with deionized water or CaCO3 saturated solution results in preferential dissolution Na2U2O7(am) and formation of schoepite. Leaching of the residual wastes with Ca(OH)2 saturated solution appears to result in transformation of both NaUO2PO4·xH2O and Na2U2O7(am) to CaUO4. Upon the basis of these results, the paragenetic sequence of secondary phases expected to occur as leaching of residual waste progresses for two tank closure scenarios was identified.</abstract><cop>Washington, DC</cop><pub>American Chemical Society</pub><pmid>21268633</pmid><doi>10.1021/es1038968</doi><tpages>8</tpages></addata></record> |
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| ispartof | Environmental science & technology, 2011-02, Vol.45 (4), p.1473-1480 |
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| subjects | Applied sciences CLOSURES DESIGN Earth sciences Earth, ocean, space Engineering and environment geology. Geothermics Environmental Modeling Environmental science ENVIRONMENTAL SCIENCES Exact sciences and technology Hanford tank residual waste LEACHING Models, Theoretical Pollution Pollution, environment geology Radioactive Waste - analysis Radioactive wastes SENSITIVITY SIMULATION single-shell tanks SOLUBILITY TANKS TESTING THERMODYNAMIC MODEL THERMODYNAMICS U solubility URANIUM Uranium - analysis Waste materials WASTES WATER X-RAY DIFFRACTION |
| title | Thermodynamic Model for Uranium Release from Hanford Site Tank Residual Waste |
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