Nitrate-Stimulated Release of Naturally Occurring Sedimentary Uranium
Groundwater uranium (U) concentrations have been measured above the U.S. EPA maximum contaminant level (30 μg/L) in many U.S. aquifers, including in areas not associated with anthropogenic contamination by milling or mining. In addition to carbonate, nitrate has been correlated to uranium groundwate...
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| Veröffentlicht in: | Environmental science & technology 2023-03, Vol.57 (10), p.4354-4366 |
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| creator | Westrop, Jeffrey P. Yadav, Pooja Nolan, PJ Campbell, Kate M. Singh, Rajesh Bone, Sharon E. Chan, Alicia H. Kohtz, Anthony J. Pan, Donald Healy, Olivia Bargar, John R. Snow, Daniel D. Weber, Karrie A. |
| description | Groundwater uranium (U) concentrations have been measured above the U.S. EPA maximum contaminant level (30 μg/L) in many U.S. aquifers, including in areas not associated with anthropogenic contamination by milling or mining. In addition to carbonate, nitrate has been correlated to uranium groundwater concentrations in two major U.S. aquifers. However, to date, direct evidence that nitrate mobilizes naturally occurring U from aquifer sediments has not been presented. Here, we demonstrate that the influx of high-nitrate porewater through High Plains alluvial aquifer silt sediments bearing naturally occurring U(IV) can stimulate a nitrate-reducing microbial community capable of catalyzing the oxidation and mobilization of U into the porewater. Microbial reduction of nitrate yielded nitrite, a reactive intermediate, which was further demonstrated to abiotically mobilize U from the reduced alluvial aquifer sediments. These results indicate that microbial activity, specifically nitrate reduction to nitrite, is one mechanism driving U mobilization from aquifer sediments in addition to previously described bicarbonate-driven desorption from mineral surfaces, such as Fe(III) oxides. |
| doi_str_mv | 10.1021/acs.est.2c07683 |
| format | Article |
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In addition to carbonate, nitrate has been correlated to uranium groundwater concentrations in two major U.S. aquifers. However, to date, direct evidence that nitrate mobilizes naturally occurring U from aquifer sediments has not been presented. Here, we demonstrate that the influx of high-nitrate porewater through High Plains alluvial aquifer silt sediments bearing naturally occurring U(IV) can stimulate a nitrate-reducing microbial community capable of catalyzing the oxidation and mobilization of U into the porewater. Microbial reduction of nitrate yielded nitrite, a reactive intermediate, which was further demonstrated to abiotically mobilize U from the reduced alluvial aquifer sediments. These results indicate that microbial activity, specifically nitrate reduction to nitrite, is one mechanism driving U mobilization from aquifer sediments in addition to previously described bicarbonate-driven desorption from mineral surfaces, such as Fe(III) oxides.</description><identifier>ISSN: 0013-936X</identifier><identifier>EISSN: 1520-5851</identifier><identifier>DOI: 10.1021/acs.est.2c07683</identifier><identifier>PMID: 36848522</identifier><language>eng</language><publisher>United States: American Chemical Society</publisher><subject>Alluvial aquifers ; Alluvial deposits ; Alluvial plains ; Anthropogenic factors ; Aquifers ; Bicarbonates ; Biogeochemical Cycling ; Biological activity ; Contaminants ; Ferric Compounds ; Geologic Sediments ; Groundwater ; High plains ; Iron ; Microbial activity ; Microorganisms ; Nitrate reduction ; Nitrates ; Nitrites ; Oxidation ; Pore water ; Reduction ; Sediments ; Uranium ; Water Pollutants, Radioactive - analysis</subject><ispartof>Environmental science & technology, 2023-03, Vol.57 (10), p.4354-4366</ispartof><rights>2023 American Chemical Society</rights><rights>Copyright American Chemical Society Mar 14, 2023</rights><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-a429t-80eacfd523e6a0e4a55141b50ebebc450fbb97a605ef3662b8aad1cfa79c8d703</citedby><cites>FETCH-LOGICAL-a429t-80eacfd523e6a0e4a55141b50ebebc450fbb97a605ef3662b8aad1cfa79c8d703</cites><orcidid>0000-0002-0457-658X ; 0000-0001-9303-4901 ; 0000-0002-8715-5544 ; 0000-0002-7521-9627 ; 0000000287155544 ; 0000000193034901 ; 000000020457658X ; 0000000275219627</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://pubs.acs.org/doi/pdf/10.1021/acs.est.2c07683$$EPDF$$P50$$Gacs$$H</linktopdf><linktohtml>$$Uhttps://pubs.acs.org/doi/10.1021/acs.est.2c07683$$EHTML$$P50$$Gacs$$H</linktohtml><link.rule.ids>230,314,776,780,881,2752,27053,27901,27902,56713,56763</link.rule.ids><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/36848522$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink><backlink>$$Uhttps://www.osti.gov/biblio/2006852$$D View this record in Osti.gov$$Hfree_for_read</backlink></links><search><creatorcontrib>Westrop, Jeffrey P.</creatorcontrib><creatorcontrib>Yadav, Pooja</creatorcontrib><creatorcontrib>Nolan, PJ</creatorcontrib><creatorcontrib>Campbell, Kate M.</creatorcontrib><creatorcontrib>Singh, Rajesh</creatorcontrib><creatorcontrib>Bone, Sharon E.</creatorcontrib><creatorcontrib>Chan, Alicia H.</creatorcontrib><creatorcontrib>Kohtz, Anthony J.</creatorcontrib><creatorcontrib>Pan, Donald</creatorcontrib><creatorcontrib>Healy, Olivia</creatorcontrib><creatorcontrib>Bargar, John R.</creatorcontrib><creatorcontrib>Snow, Daniel D.</creatorcontrib><creatorcontrib>Weber, Karrie A.</creatorcontrib><creatorcontrib>SLAC</creatorcontrib><title>Nitrate-Stimulated Release of Naturally Occurring Sedimentary Uranium</title><title>Environmental science & technology</title><addtitle>Environ. 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Sci. Technol</addtitle><date>2023-03-14</date><risdate>2023</risdate><volume>57</volume><issue>10</issue><spage>4354</spage><epage>4366</epage><pages>4354-4366</pages><issn>0013-936X</issn><eissn>1520-5851</eissn><abstract>Groundwater uranium (U) concentrations have been measured above the U.S. EPA maximum contaminant level (30 μg/L) in many U.S. aquifers, including in areas not associated with anthropogenic contamination by milling or mining. In addition to carbonate, nitrate has been correlated to uranium groundwater concentrations in two major U.S. aquifers. However, to date, direct evidence that nitrate mobilizes naturally occurring U from aquifer sediments has not been presented. Here, we demonstrate that the influx of high-nitrate porewater through High Plains alluvial aquifer silt sediments bearing naturally occurring U(IV) can stimulate a nitrate-reducing microbial community capable of catalyzing the oxidation and mobilization of U into the porewater. Microbial reduction of nitrate yielded nitrite, a reactive intermediate, which was further demonstrated to abiotically mobilize U from the reduced alluvial aquifer sediments. These results indicate that microbial activity, specifically nitrate reduction to nitrite, is one mechanism driving U mobilization from aquifer sediments in addition to previously described bicarbonate-driven desorption from mineral surfaces, such as Fe(III) oxides.</abstract><cop>United States</cop><pub>American Chemical Society</pub><pmid>36848522</pmid><doi>10.1021/acs.est.2c07683</doi><tpages>13</tpages><orcidid>https://orcid.org/0000-0002-0457-658X</orcidid><orcidid>https://orcid.org/0000-0001-9303-4901</orcidid><orcidid>https://orcid.org/0000-0002-8715-5544</orcidid><orcidid>https://orcid.org/0000-0002-7521-9627</orcidid><orcidid>https://orcid.org/0000000287155544</orcidid><orcidid>https://orcid.org/0000000193034901</orcidid><orcidid>https://orcid.org/000000020457658X</orcidid><orcidid>https://orcid.org/0000000275219627</orcidid><oa>free_for_read</oa></addata></record> |
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| source | ACS Publications; MEDLINE |
| subjects | Alluvial aquifers Alluvial deposits Alluvial plains Anthropogenic factors Aquifers Bicarbonates Biogeochemical Cycling Biological activity Contaminants Ferric Compounds Geologic Sediments Groundwater High plains Iron Microbial activity Microorganisms Nitrate reduction Nitrates Nitrites Oxidation Pore water Reduction Sediments Uranium Water Pollutants, Radioactive - analysis |
| title | Nitrate-Stimulated Release of Naturally Occurring Sedimentary Uranium |
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