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Multiple Lines of Evidence Identify U(V) as a Key Intermediate during U(VI) Reduction by MR1

Vettese, Gianni F.; Morris, Katherine; Natrajan, Louise S.; Shaw, Samuel; Vitova, Tonya ORCID iD icon 1; Galanzew, Jurij 1; Jones, Debbie L.; Lloyd, Jonathan R.
1 Institut für Nukleare Entsorgung (INE), Karlsruher Institut für Technologie (KIT)

Abstract:

As the dominant radionuclide by mass in many radioactive wastes, the control of uranium mobility in contaminated environments is of high concern. U speciation can be governed by microbial interactions, whereby metal-reducing bacteria are able to reduce soluble U(VI) to insoluble U(IV), providing a method for removal of U from contaminated groundwater. Although microbial U(VI) reduction is widely reported, the mechanism(s) for the transformation of U(VI) to relatively insoluble U(IV) phases are poorly understood. By combining a suite of analyses, including luminescence, U M$_{4}$-edge high-energy resolved fluorescence detection–X-ray absorption near-edge structure (XANES), and U L$_{3}$-edge XANES/extended X-ray absorption fine structure, we show that the microbial reduction of U(VI) by the model Fe(III)-reducing bacterium, Shewanella oneidensis MR1, proceeds via a single electron transfer to form a pentavalent U(V) intermediate which disproportionates to form U(VI) and U(IV). Furthermore, we have identified significant U(V) present in post reduction solid phases, implying that U(V) may be stabilized for up to 120.5 h.


Verlagsausgabe §
DOI: 10.5445/IR/1000118132
Veröffentlicht am 28.11.2021
Originalveröffentlichung
DOI: 10.1021/acs.est.9b05285
Scopus
Zitationen: 25
Web of Science
Zitationen: 24
Dimensions
Zitationen: 31
Cover der Publikation
Zugehörige Institution(en) am KIT Institut für Nukleare Entsorgung (INE)
Publikationstyp Zeitschriftenaufsatz
Publikationsdatum 18.02.2020
Sprache Englisch
Identifikator ISSN: 0013-936X, 1520-5851
KITopen-ID: 1000118132
HGF-Programm 32.01.04 (POF III, LK 01) Entw.u.Anpassung v.Speziationsmethoden
Weitere HGF-Programme 54.11.11 (POF IV, LK 01) Accelerator Operation, Research and Development
Erschienen in Environmental science & technology
Verlag American Chemical Society (ACS)
Band 54
Heft 4
Seiten 2268–2276
Vorab online veröffentlicht am 14.01.2020
Nachgewiesen in Dimensions
Web of Science
Scopus
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