Pore-scale evaluation of uranyl phosphate precipitation in a model groundwater system
Key Points In situ uranyl phosphate precipitation is fast on the time scale of remediation Ca2+ & SO42‐ affect uranyl phosphate precipitation rate and morphology Only chernikovite is formed, and it blocks pore spaces and reduces mixing The abiotic precipitation of uranium (U(VI)) was evaluated i...
Gespeichert in:
| Veröffentlicht in: | Water Resources Research, 49(2):874-890 49(2):874-890, 2013-02, Vol.49 (2), p.874-890 |
|---|---|
| Hauptverfasser: | , , , , , , , , , |
| Format: | Artikel |
| Sprache: | eng |
| Schlagworte: | |
| Online-Zugang: | Volltext |
| Tags: |
Tag hinzufügen
Keine Tags, Fügen Sie den ersten Tag hinzu!
|
| container_end_page | 890 |
|---|---|
| container_issue | 2 |
| container_start_page | 874 |
| container_title | Water Resources Research, 49(2):874-890 |
| container_volume | 49 |
| creator | Fanizza, Michael F. Yoon, Hongkyu Zhang, Changyong Oostrom, Martinus Wietsma, Thomas W. Hess, Nancy J. Bowden, Mark E. Strathmann, Timothy J. Finneran, Kevin T. Werth, Charles J. |
| description | Key Points
In situ uranyl phosphate precipitation is fast on the time scale of remediation
Ca2+ & SO42‐ affect uranyl phosphate precipitation rate and morphology
Only chernikovite is formed, and it blocks pore spaces and reduces mixing
The abiotic precipitation of uranium (U(VI)) was evaluated in a microfluidic pore network (i.e., micromodel) to assess the efficacy of using a phosphate amendment to immobilize uranium in groundwater. U(VI) was mixed transverse to the direction of flow with hydrogen phosphate (HPO42−), in the presence or absence of calcium (Ca2+) or sulfate (SO42−), in order to identify precipitation rates, morphology and types of minerals formed, and effects of mineral precipitates on pore blockage. Precipitation occurred over the time scale of hours to days. Relative to when only U(VI) and HPO42− were present, precipitation rates were 2.3 times slower when SO42− was present, and 1.4 times faster when Ca2+ was present; larger crystals formed in the presence of SO42−. Raman backscattering spectroscopy and micro‐X‐ray diffraction results both showed that the only mineral precipitated was chernikovite, UO2HPO4 · 4H2O; energy dispersive X‐ray spectroscopy results indicate that Ca and S are not incorporated into the chernikovite lattice. A pore‐scale model was developed, and simulation results of saturation ratio (SR = Q/Ksp) suggest that chernikovite is the least thermodynamically favored mineral to precipitate (0 < SR < 1) compared to uranyl hydrogen phosphate and Na‐autunite (13 < SR < 40), and uranyl orthophosphate and Ca‐autunite (when Ca2+ is present; SR > 105). Fluorescent tracer studies and laser confocal microscopy images showed that densely aggregated precipitates blocked pores and reduced permeability. The results suggest that uranium precipitation with phosphate as chernikovite is rapid on the time scale of remediation for the conditions considered and can block pores, alter fluid flow paths, and potentially limit mixing and precipitation. |
| doi_str_mv | 10.1002/wrcr.20088 |
| format | Article |
| fullrecord | <record><control><sourceid>proquest_osti_</sourceid><recordid>TN_cdi_proquest_miscellaneous_1566842706</recordid><sourceformat>XML</sourceformat><sourcesystem>PC</sourcesystem><sourcerecordid>1566842706</sourcerecordid><originalsourceid>FETCH-LOGICAL-a5248-3f8e996645ff710e19a5cdab3acb8116b25ba7f55403bc2ffc5bd7a2c585d6703</originalsourceid><addsrcrecordid>eNp90c1u1DAUBWCrAqlDYcMTWO0GIaXY8V-yRAOUojKgijJSN5bjXHfcZuJgJ0zn7XFJYcGClTffsa_vQeglJaeUkPLNLtp4WhJSVQdoQWvOC1Ur9gQtCOGsoKxWh-hZSreEUC6kWqCrryFCkazpAMNP001m9KHHweEpmn7f4WET0rAxI-AhgvWDH2fhe2zwNrTQ4ZsYpr7dZRNx2qcRts_RU2e6BC8ezyN09eH9t-XH4uLL2fny7UVhRMmrgrkK6lpKLpxTlACtjbCtaZixTUWpbErRGOWE4IQ1tnTOiqZVprSiEq1UhB2h4_nekEavk_Uj2I0NfQ921JQoKVWV0asZDTH8mCCNeuuTha4zPYQpaSqkrHipiMz05B96G6bY5y9oKnlJ8lCszur1rGwMKUVweoh-a-I-P6kfatAPNejfNWRMZ7zzHez_I_X6cnn5J1PMGZ-Xef83Y-KdloopoderM00_ff-8ul6902v2C4t9miY</addsrcrecordid><sourcetype>Open Access Repository</sourcetype><iscdi>true</iscdi><recordtype>article</recordtype><pqid>1642081139</pqid></control><display><type>article</type><title>Pore-scale evaluation of uranyl phosphate precipitation in a model groundwater system</title><source>Access via Wiley Online Library</source><source>Wiley-Blackwell AGU Digital Library</source><source>EZB-FREE-00999 freely available EZB journals</source><creator>Fanizza, Michael F. ; Yoon, Hongkyu ; Zhang, Changyong ; Oostrom, Martinus ; Wietsma, Thomas W. ; Hess, Nancy J. ; Bowden, Mark E. ; Strathmann, Timothy J. ; Finneran, Kevin T. ; Werth, Charles J.</creator><creatorcontrib>Fanizza, Michael F. ; Yoon, Hongkyu ; Zhang, Changyong ; Oostrom, Martinus ; Wietsma, Thomas W. ; Hess, Nancy J. ; Bowden, Mark E. ; Strathmann, Timothy J. ; Finneran, Kevin T. ; Werth, Charles J. ; Pacific Northwest National Laboratory (PNNL), Richland, WA (US), Environmental Molecular Sciences Laboratory (EMSL)</creatorcontrib><description>Key Points
In situ uranyl phosphate precipitation is fast on the time scale of remediation
Ca2+ & SO42‐ affect uranyl phosphate precipitation rate and morphology
Only chernikovite is formed, and it blocks pore spaces and reduces mixing
The abiotic precipitation of uranium (U(VI)) was evaluated in a microfluidic pore network (i.e., micromodel) to assess the efficacy of using a phosphate amendment to immobilize uranium in groundwater. U(VI) was mixed transverse to the direction of flow with hydrogen phosphate (HPO42−), in the presence or absence of calcium (Ca2+) or sulfate (SO42−), in order to identify precipitation rates, morphology and types of minerals formed, and effects of mineral precipitates on pore blockage. Precipitation occurred over the time scale of hours to days. Relative to when only U(VI) and HPO42− were present, precipitation rates were 2.3 times slower when SO42− was present, and 1.4 times faster when Ca2+ was present; larger crystals formed in the presence of SO42−. Raman backscattering spectroscopy and micro‐X‐ray diffraction results both showed that the only mineral precipitated was chernikovite, UO2HPO4 · 4H2O; energy dispersive X‐ray spectroscopy results indicate that Ca and S are not incorporated into the chernikovite lattice. A pore‐scale model was developed, and simulation results of saturation ratio (SR = Q/Ksp) suggest that chernikovite is the least thermodynamically favored mineral to precipitate (0 < SR < 1) compared to uranyl hydrogen phosphate and Na‐autunite (13 < SR < 40), and uranyl orthophosphate and Ca‐autunite (when Ca2+ is present; SR > 105). Fluorescent tracer studies and laser confocal microscopy images showed that densely aggregated precipitates blocked pores and reduced permeability. The results suggest that uranium precipitation with phosphate as chernikovite is rapid on the time scale of remediation for the conditions considered and can block pores, alter fluid flow paths, and potentially limit mixing and precipitation.</description><identifier>ISSN: 0043-1397</identifier><identifier>EISSN: 1944-7973</identifier><identifier>DOI: 10.1002/wrcr.20088</identifier><language>eng</language><publisher>Washington: Blackwell Publishing Ltd</publisher><subject>Crystals ; Environmental Molecular Sciences Laboratory ; Fluid flow ; mixing ; Morphology ; pore scale ; Pores ; precipitation ; Spectrum analysis ; Uranium ; X-ray diffraction ; X-ray spectroscopy</subject><ispartof>Water Resources Research, 49(2):874-890, 2013-02, Vol.49 (2), p.874-890</ispartof><rights>2013. American Geophysical Union. All Rights Reserved.</rights><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-a5248-3f8e996645ff710e19a5cdab3acb8116b25ba7f55403bc2ffc5bd7a2c585d6703</citedby><cites>FETCH-LOGICAL-a5248-3f8e996645ff710e19a5cdab3acb8116b25ba7f55403bc2ffc5bd7a2c585d6703</cites></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://onlinelibrary.wiley.com/doi/pdf/10.1002%2Fwrcr.20088$$EPDF$$P50$$Gwiley$$H</linktopdf><linktohtml>$$Uhttps://onlinelibrary.wiley.com/doi/full/10.1002%2Fwrcr.20088$$EHTML$$P50$$Gwiley$$H</linktohtml><link.rule.ids>314,780,784,885,1417,11514,27924,27925,45574,45575,46468,46892</link.rule.ids><backlink>$$Uhttps://www.osti.gov/biblio/1076678$$D View this record in Osti.gov$$Hfree_for_read</backlink></links><search><creatorcontrib>Fanizza, Michael F.</creatorcontrib><creatorcontrib>Yoon, Hongkyu</creatorcontrib><creatorcontrib>Zhang, Changyong</creatorcontrib><creatorcontrib>Oostrom, Martinus</creatorcontrib><creatorcontrib>Wietsma, Thomas W.</creatorcontrib><creatorcontrib>Hess, Nancy J.</creatorcontrib><creatorcontrib>Bowden, Mark E.</creatorcontrib><creatorcontrib>Strathmann, Timothy J.</creatorcontrib><creatorcontrib>Finneran, Kevin T.</creatorcontrib><creatorcontrib>Werth, Charles J.</creatorcontrib><creatorcontrib>Pacific Northwest National Laboratory (PNNL), Richland, WA (US), Environmental Molecular Sciences Laboratory (EMSL)</creatorcontrib><title>Pore-scale evaluation of uranyl phosphate precipitation in a model groundwater system</title><title>Water Resources Research, 49(2):874-890</title><addtitle>Water Resour. Res</addtitle><description>Key Points
In situ uranyl phosphate precipitation is fast on the time scale of remediation
Ca2+ & SO42‐ affect uranyl phosphate precipitation rate and morphology
Only chernikovite is formed, and it blocks pore spaces and reduces mixing
The abiotic precipitation of uranium (U(VI)) was evaluated in a microfluidic pore network (i.e., micromodel) to assess the efficacy of using a phosphate amendment to immobilize uranium in groundwater. U(VI) was mixed transverse to the direction of flow with hydrogen phosphate (HPO42−), in the presence or absence of calcium (Ca2+) or sulfate (SO42−), in order to identify precipitation rates, morphology and types of minerals formed, and effects of mineral precipitates on pore blockage. Precipitation occurred over the time scale of hours to days. Relative to when only U(VI) and HPO42− were present, precipitation rates were 2.3 times slower when SO42− was present, and 1.4 times faster when Ca2+ was present; larger crystals formed in the presence of SO42−. Raman backscattering spectroscopy and micro‐X‐ray diffraction results both showed that the only mineral precipitated was chernikovite, UO2HPO4 · 4H2O; energy dispersive X‐ray spectroscopy results indicate that Ca and S are not incorporated into the chernikovite lattice. A pore‐scale model was developed, and simulation results of saturation ratio (SR = Q/Ksp) suggest that chernikovite is the least thermodynamically favored mineral to precipitate (0 < SR < 1) compared to uranyl hydrogen phosphate and Na‐autunite (13 < SR < 40), and uranyl orthophosphate and Ca‐autunite (when Ca2+ is present; SR > 105). Fluorescent tracer studies and laser confocal microscopy images showed that densely aggregated precipitates blocked pores and reduced permeability. The results suggest that uranium precipitation with phosphate as chernikovite is rapid on the time scale of remediation for the conditions considered and can block pores, alter fluid flow paths, and potentially limit mixing and precipitation.</description><subject>Crystals</subject><subject>Environmental Molecular Sciences Laboratory</subject><subject>Fluid flow</subject><subject>mixing</subject><subject>Morphology</subject><subject>pore scale</subject><subject>Pores</subject><subject>precipitation</subject><subject>Spectrum analysis</subject><subject>Uranium</subject><subject>X-ray diffraction</subject><subject>X-ray spectroscopy</subject><issn>0043-1397</issn><issn>1944-7973</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2013</creationdate><recordtype>article</recordtype><recordid>eNp90c1u1DAUBWCrAqlDYcMTWO0GIaXY8V-yRAOUojKgijJSN5bjXHfcZuJgJ0zn7XFJYcGClTffsa_vQeglJaeUkPLNLtp4WhJSVQdoQWvOC1Ur9gQtCOGsoKxWh-hZSreEUC6kWqCrryFCkazpAMNP001m9KHHweEpmn7f4WET0rAxI-AhgvWDH2fhe2zwNrTQ4ZsYpr7dZRNx2qcRts_RU2e6BC8ezyN09eH9t-XH4uLL2fny7UVhRMmrgrkK6lpKLpxTlACtjbCtaZixTUWpbErRGOWE4IQ1tnTOiqZVprSiEq1UhB2h4_nekEavk_Uj2I0NfQ921JQoKVWV0asZDTH8mCCNeuuTha4zPYQpaSqkrHipiMz05B96G6bY5y9oKnlJ8lCszur1rGwMKUVweoh-a-I-P6kfatAPNejfNWRMZ7zzHez_I_X6cnn5J1PMGZ-Xef83Y-KdloopoderM00_ff-8ul6902v2C4t9miY</recordid><startdate>201302</startdate><enddate>201302</enddate><creator>Fanizza, Michael F.</creator><creator>Yoon, Hongkyu</creator><creator>Zhang, Changyong</creator><creator>Oostrom, Martinus</creator><creator>Wietsma, Thomas W.</creator><creator>Hess, Nancy J.</creator><creator>Bowden, Mark E.</creator><creator>Strathmann, Timothy J.</creator><creator>Finneran, Kevin T.</creator><creator>Werth, Charles J.</creator><general>Blackwell Publishing Ltd</general><general>John Wiley & Sons, Inc</general><scope>BSCLL</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>7QH</scope><scope>7QL</scope><scope>7T7</scope><scope>7TG</scope><scope>7U9</scope><scope>7UA</scope><scope>8FD</scope><scope>C1K</scope><scope>F1W</scope><scope>FR3</scope><scope>H94</scope><scope>H96</scope><scope>KL.</scope><scope>KR7</scope><scope>L.G</scope><scope>M7N</scope><scope>P64</scope><scope>7TV</scope><scope>H97</scope><scope>OTOTI</scope></search><sort><creationdate>201302</creationdate><title>Pore-scale evaluation of uranyl phosphate precipitation in a model groundwater system</title><author>Fanizza, Michael F. ; Yoon, Hongkyu ; Zhang, Changyong ; Oostrom, Martinus ; Wietsma, Thomas W. ; Hess, Nancy J. ; Bowden, Mark E. ; Strathmann, Timothy J. ; Finneran, Kevin T. ; Werth, Charles J.</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-a5248-3f8e996645ff710e19a5cdab3acb8116b25ba7f55403bc2ffc5bd7a2c585d6703</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2013</creationdate><topic>Crystals</topic><topic>Environmental Molecular Sciences Laboratory</topic><topic>Fluid flow</topic><topic>mixing</topic><topic>Morphology</topic><topic>pore scale</topic><topic>Pores</topic><topic>precipitation</topic><topic>Spectrum analysis</topic><topic>Uranium</topic><topic>X-ray diffraction</topic><topic>X-ray spectroscopy</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Fanizza, Michael F.</creatorcontrib><creatorcontrib>Yoon, Hongkyu</creatorcontrib><creatorcontrib>Zhang, Changyong</creatorcontrib><creatorcontrib>Oostrom, Martinus</creatorcontrib><creatorcontrib>Wietsma, Thomas W.</creatorcontrib><creatorcontrib>Hess, Nancy J.</creatorcontrib><creatorcontrib>Bowden, Mark E.</creatorcontrib><creatorcontrib>Strathmann, Timothy J.</creatorcontrib><creatorcontrib>Finneran, Kevin T.</creatorcontrib><creatorcontrib>Werth, Charles J.</creatorcontrib><creatorcontrib>Pacific Northwest National Laboratory (PNNL), Richland, WA (US), Environmental Molecular Sciences Laboratory (EMSL)</creatorcontrib><collection>Istex</collection><collection>CrossRef</collection><collection>Aqualine</collection><collection>Bacteriology Abstracts (Microbiology B)</collection><collection>Industrial and Applied Microbiology Abstracts (Microbiology A)</collection><collection>Meteorological & Geoastrophysical Abstracts</collection><collection>Virology and AIDS Abstracts</collection><collection>Water Resources Abstracts</collection><collection>Technology Research Database</collection><collection>Environmental Sciences and Pollution Management</collection><collection>ASFA: Aquatic Sciences and Fisheries Abstracts</collection><collection>Engineering Research Database</collection><collection>AIDS and Cancer Research Abstracts</collection><collection>Aquatic Science & Fisheries Abstracts (ASFA) 2: Ocean Technology, Policy & Non-Living Resources</collection><collection>Meteorological & Geoastrophysical Abstracts - Academic</collection><collection>Civil Engineering Abstracts</collection><collection>Aquatic Science & Fisheries Abstracts (ASFA) Professional</collection><collection>Algology Mycology and Protozoology Abstracts (Microbiology C)</collection><collection>Biotechnology and BioEngineering Abstracts</collection><collection>Pollution Abstracts</collection><collection>Aquatic Science & Fisheries Abstracts (ASFA) 3: Aquatic Pollution & Environmental Quality</collection><collection>OSTI.GOV</collection><jtitle>Water Resources Research, 49(2):874-890</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Fanizza, Michael F.</au><au>Yoon, Hongkyu</au><au>Zhang, Changyong</au><au>Oostrom, Martinus</au><au>Wietsma, Thomas W.</au><au>Hess, Nancy J.</au><au>Bowden, Mark E.</au><au>Strathmann, Timothy J.</au><au>Finneran, Kevin T.</au><au>Werth, Charles J.</au><aucorp>Pacific Northwest National Laboratory (PNNL), Richland, WA (US), Environmental Molecular Sciences Laboratory (EMSL)</aucorp><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Pore-scale evaluation of uranyl phosphate precipitation in a model groundwater system</atitle><jtitle>Water Resources Research, 49(2):874-890</jtitle><addtitle>Water Resour. Res</addtitle><date>2013-02</date><risdate>2013</risdate><volume>49</volume><issue>2</issue><spage>874</spage><epage>890</epage><pages>874-890</pages><issn>0043-1397</issn><eissn>1944-7973</eissn><abstract>Key Points
In situ uranyl phosphate precipitation is fast on the time scale of remediation
Ca2+ & SO42‐ affect uranyl phosphate precipitation rate and morphology
Only chernikovite is formed, and it blocks pore spaces and reduces mixing
The abiotic precipitation of uranium (U(VI)) was evaluated in a microfluidic pore network (i.e., micromodel) to assess the efficacy of using a phosphate amendment to immobilize uranium in groundwater. U(VI) was mixed transverse to the direction of flow with hydrogen phosphate (HPO42−), in the presence or absence of calcium (Ca2+) or sulfate (SO42−), in order to identify precipitation rates, morphology and types of minerals formed, and effects of mineral precipitates on pore blockage. Precipitation occurred over the time scale of hours to days. Relative to when only U(VI) and HPO42− were present, precipitation rates were 2.3 times slower when SO42− was present, and 1.4 times faster when Ca2+ was present; larger crystals formed in the presence of SO42−. Raman backscattering spectroscopy and micro‐X‐ray diffraction results both showed that the only mineral precipitated was chernikovite, UO2HPO4 · 4H2O; energy dispersive X‐ray spectroscopy results indicate that Ca and S are not incorporated into the chernikovite lattice. A pore‐scale model was developed, and simulation results of saturation ratio (SR = Q/Ksp) suggest that chernikovite is the least thermodynamically favored mineral to precipitate (0 < SR < 1) compared to uranyl hydrogen phosphate and Na‐autunite (13 < SR < 40), and uranyl orthophosphate and Ca‐autunite (when Ca2+ is present; SR > 105). Fluorescent tracer studies and laser confocal microscopy images showed that densely aggregated precipitates blocked pores and reduced permeability. The results suggest that uranium precipitation with phosphate as chernikovite is rapid on the time scale of remediation for the conditions considered and can block pores, alter fluid flow paths, and potentially limit mixing and precipitation.</abstract><cop>Washington</cop><pub>Blackwell Publishing Ltd</pub><doi>10.1002/wrcr.20088</doi><tpages>17</tpages><oa>free_for_read</oa></addata></record> |
| fulltext | fulltext |
| identifier | ISSN: 0043-1397 |
| ispartof | Water Resources Research, 49(2):874-890, 2013-02, Vol.49 (2), p.874-890 |
| issn | 0043-1397 1944-7973 |
| language | eng |
| recordid | cdi_proquest_miscellaneous_1566842706 |
| source | Access via Wiley Online Library; Wiley-Blackwell AGU Digital Library; EZB-FREE-00999 freely available EZB journals |
| subjects | Crystals Environmental Molecular Sciences Laboratory Fluid flow mixing Morphology pore scale Pores precipitation Spectrum analysis Uranium X-ray diffraction X-ray spectroscopy |
| title | Pore-scale evaluation of uranyl phosphate precipitation in a model groundwater system |
| url | https://sfx.bib-bvb.de/sfx_tum?ctx_ver=Z39.88-2004&ctx_enc=info:ofi/enc:UTF-8&ctx_tim=2024-12-23T03%3A08%3A28IST&url_ver=Z39.88-2004&url_ctx_fmt=infofi/fmt:kev:mtx:ctx&rfr_id=info:sid/primo.exlibrisgroup.com:primo3-Article-proquest_osti_&rft_val_fmt=info:ofi/fmt:kev:mtx:journal&rft.genre=article&rft.atitle=Pore-scale%20evaluation%20of%20uranyl%20phosphate%20precipitation%20in%20a%20model%20groundwater%20system&rft.jtitle=Water%20Resources%20Research,%2049(2):874-890&rft.au=Fanizza,%20Michael%20F.&rft.aucorp=Pacific%20Northwest%20National%20Laboratory%20(PNNL),%20Richland,%20WA%20(US),%20Environmental%20Molecular%20Sciences%20Laboratory%20(EMSL)&rft.date=2013-02&rft.volume=49&rft.issue=2&rft.spage=874&rft.epage=890&rft.pages=874-890&rft.issn=0043-1397&rft.eissn=1944-7973&rft_id=info:doi/10.1002/wrcr.20088&rft_dat=%3Cproquest_osti_%3E1566842706%3C/proquest_osti_%3E%3Curl%3E%3C/url%3E&disable_directlink=true&sfx.directlink=off&sfx.report_link=0&rft_id=info:oai/&rft_pqid=1642081139&rft_id=info:pmid/&rfr_iscdi=true |