Sulfidation of magnetite with incorporated uranium

Townsend, Luke; Morris, Katherine; Harrison, Robert; Schacherl, Bianca; Vitova, Tonya; Kovarik, Libor; Pearce, Carolyn I.; Mosselmans, JFW; Shaw, Samuel

doi:10.1016/j.chemosphere.2021.130117

Sulfidation of magnetite with incorporated uranium

Journal Article · 02 August 2021 · Chemosphere

DOI:https://doi.org/10.1016/j.chemosphere.2021.130117· OSTI ID:1772344

Townsend, Luke ^[1]; Morris, Katherine ^[1]; Harrison, Robert ^[1]; Schacherl, Bianca ^[2]; Vitova, Tonya ^[2]; Kovarik, Libor ^[3]; Pearce, Carolyn I. ^[3]; Mosselmans, JFW ^[4]; Shaw, Samuel ^[1]

University of Manchester
Institute for Nuclear Waste Disposal
BATTELLE (PACIFIC NW LAB)
Diamond Light Source

Uranium (U) is a radionuclide of key environmental interest due its abundance by mass within radioactive waste and presence in contaminated land scenarios. Ubiquitously present iron (oxyhydr)oxide mineral phases, such as (nano)magnetite, have been identified as candidates for immobilisation of U via incorporation into the mineral structure. Studies of how biogeochemicalprocesses, such as sulfidation from the presence of sulfate-reducing bacteria, may affect iron (oxyhydr)oxides and impact radionuclide mobility are important in order to underpin geological disposal of radioactive waste and manage radioactively contaminated land. Here, this study utilised a highly controlled abiotic method for sulfidation of U(V) incorporated into nanomagnetite to determine the fate and speciation of U. Upon sulfidation, transient release of U into solution occurred (~8.6 % total U) for up to 3 days, despite the highly reducing conditions. As the system evolved, lepidocrocite was observed to form over a period of days to weeks. After 10 months, XAS and geochemical data showed all U was partitioned to the solid phase, as both nanoparticulate uraninite (U(IV)O2) and a percentage of retained U(V). Further EXAFS analysis showed incorporation of the residual U(V) fraction into an iron (oxyhydr)oxide mineral phase, likely nanomagnetite or lepidocrocite. Overall, these results provide new insights into the stability of U(V) incorporated iron (oxyhydr)oxides during sulfidation, confirming the longer term retention of U in the solid phase under complex, environmentally relevant conditions.

Research Organization:: Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE

DOE Contract Number:: AC05-76RL01830

OSTI ID:: 1772344

Report Number(s):: PNNL-SA-160714

Journal Information:: Chemosphere, Vol. 276

Country of Publication:: United States

Language:: English

References (67)

Quantitative Separation of Monomeric U(IV) from UO ₂ in Products of U(VI) Reduction Alessi, Daniel S.; Uster, Benjamin; Veeramani, Harish Environmental Science & Technology, Vol. 46, Issue 11 https://doi.org/10.1021/es204123z	journal	May 2012
The product of microbial uranium reduction includes multiple species with U(IV)–phosphate coordination Alessi, Daniel S.; Lezama-Pacheco, Juan S.; Stubbs, Joanne E. Geochimica et Cosmochimica Acta, Vol. 131 https://doi.org/10.1016/j.gca.2014.01.005	journal	April 2014
Sulfidization of lepidocrocite and its effect on uranium phase distribution and reduction Alexandratos, Vasso G.; Behrends, Thilo; Van Cappellen, Philippe Geochimica et Cosmochimica Acta, Vol. 142 https://doi.org/10.1016/j.gca.2014.08.009	journal	October 2014
Fate of Adsorbed U(VI) during Sulfidization of Lepidocrocite and Hematite Alexandratos, Vasso G.; Behrends, Thilo; Van Cappellen, Philippe Environmental Science & Technology, Vol. 51, Issue 4 https://doi.org/10.1021/acs.est.6b05453	journal	February 2017
Stimulating the In Situ Activity of Geobacter Species To Remove Uranium from the Groundwater of a Uranium-Contaminated Aquifer Anderson, R. T.; Vrionis, H. A.; Ortiz-Bernad, I. Applied and Environmental Microbiology, Vol. 69, Issue 10 https://doi.org/10.1128/AEM.69.10.5884-5891.2003	journal	October 2003
Uranium redox transition pathways in acetate-amended sediments Bargar, J. R.; Williams, K. H.; Campbell, K. M. Proceedings of the National Academy of Sciences, Vol. 110, Issue 12 https://doi.org/10.1073/pnas.1219198110	journal	March 2013
The Presence of Sulphate Reducing Bacteria in oil Field Waters Bastin, E. S.; Greer, F. E.; Merritt, C. A. Science, Vol. 63, Issue 1618 https://doi.org/10.1126/science.63.1618.21	journal	January 1926
Geochemical controls of the microbially mediated redox cycling of uranium and iron Belli, Keaton M.; Taillefert, Martial Geochimica et Cosmochimica Acta, Vol. 235 https://doi.org/10.1016/j.gca.2018.05.027	journal	August 2018
Non-uraninite Products of Microbial U(VI) Reduction Bernier-Latmani, Rizlan; Veeramani, Harish; Vecchia, Elena Dalla Environmental Science & Technology, Vol. 44, Issue 24 https://doi.org/10.1021/es101675a	journal	December 2010
Use of HERFD–XANES at the U L ₃ - and M ₄ -Edges To Determine the Uranium Valence State on [Ni(H ₂ O) ₄ ] ₃ [U(OH,H ₂ O)(UO ₂ ) ₈ O ₁₂ (OH) ₃ ] Bès, René; Rivenet, Murielle; Solari, Pier-Lorenzo Inorganic Chemistry, Vol. 55, Issue 9 https://doi.org/10.1021/acs.inorgchem.6b00014	journal	April 2016
Standard Electrode Potentials and Temperature Coefficients in Water at 298.15 K Bratsch, Steven G. Journal of Physical and Chemical Reference Data, Vol. 18, Issue 1 https://doi.org/10.1063/1.555839	journal	January 1989
Characterization of uraninite nanoparticles produced by Shewanella oneidensis MR-1 Burgos, William D.; McDonough, Jeffrey T.; Senko, John M. Geochimica et Cosmochimica Acta, Vol. 72, Issue 20 https://doi.org/10.1016/j.gca.2008.07.016	journal	October 2008
Reactive iron in marine sediments Canfield, Donald E. Geochimica et Cosmochimica Acta, Vol. 53, Issue 3 https://doi.org/10.1016/0016-7037(89)90005-7	journal	March 1989
Dissolution and pyritization of magnetite in anoxie marine sediments Canfield, Donald E.; Berner, Robert A. Geochimica et Cosmochimica Acta, Vol. 51, Issue 3 https://doi.org/10.1016/0016-7037(87)90076-7	journal	March 1987
Mechanisms and Rates of U(VI) Reduction by Fe(II) in Homogeneous Aqueous Solution and the Role of U(V) Disproportionation Collins, Richard N.; Rosso, Kevin M. The Journal of Physical Chemistry A, Vol. 121, Issue 35 https://doi.org/10.1021/acs.jpca.7b05965	journal	August 2017
X-ray Absorption Spectroscopy of Tricarbonatodioxouranate(V), [UO ₂ (CO ₃ ) ₃ ] ⁵ ^- , in Aqueous Solution Docrat, T. I.; Mosselmans, J. F. W.; Charnock, J. M. Inorganic Chemistry, Vol. 38, Issue 8 https://doi.org/10.1021/ic9814423	journal	April 1999
Reductive dissolution of iron(III) (hydr)oxides by hydrogen sulfide Dos Santos Afonso, Maria; Stumm, Werner Langmuir, Vol. 8, Issue 6 https://doi.org/10.1021/la00042a030	journal	June 1992
Kinetics and mechanism of the disproportionation of uranium(V) Ekstrom, A. Inorganic Chemistry, Vol. 13, Issue 9 https://doi.org/10.1021/ic50139a035	journal	September 1974
Synthesis and Characterization of a Water Stable Uranyl(V) Complex Faizova, Radmila; Scopelliti, Rosario; Chauvin, Anne-Sophie Journal of the American Chemical Society, Vol. 140, Issue 42 https://doi.org/10.1021/jacs.8b07885	journal	September 2018
Organic complexation of U(VI) in reducing soils at a natural analogue site: Implications for uranium transport Fuller, Adam J.; Leary, Peter; Gray, Neil D. Chemosphere, Vol. 254 https://doi.org/10.1016/j.chemosphere.2020.126859	journal	September 2020
Uranium(VI) Interactions with Mackinawite in the Presence and Absence of Bicarbonate and Oxygen Gallegos, Tanya J.; Fuller, Christopher C.; Webb, Samuel M. Environmental Science & Technology, Vol. 47, Issue 13 https://doi.org/10.1021/es400450z	journal	June 2013
Synthesis, surface characterization and electrokinetic properties of colloidal silica nanoparticles with magnetic core Gdula, Karolina; Dąbrowski, Andrzej; Skwarek, Ewa Adsorption, Vol. 22, Issue 4-6 https://doi.org/10.1007/s10450-015-9755-8	journal	January 2016
Amine-functionalized silica particles with magnetic core as magnetically removable adsorbents of Ag(I) ions Gdula, Karolina; Skwarek, Ewa; Dąbrowski, Andrzej Adsorption Science & Technology, Vol. 35, Issue 5-6 https://doi.org/10.1177/0263617417694365	journal	January 2017
Amine-functionalized magnetite-silica nanoparticles as effective adsorbent for removal of uranium(VI) ions Gdula, Karolina; Gładysz-Płaska, Agnieszka; Cristóvão, Beata Journal of Molecular Liquids, Vol. 290 https://doi.org/10.1016/j.molliq.2019.111217	journal	September 2019
Equation of state of magnetite and its high-pressure modification: Thermodynamics of the Fe-O system at high pressure Haavik, Camilla; Stølen, Svein; Fjellvåg, Helmer American Mineralogist, Vol. 85, Issue 3-4 https://doi.org/10.2138/am-2000-0413	journal	March 2000
Pathways of ferrous iron mineral formation upon sulfidation of lepidocrocite surfaces Hellige, Katrin; Pollok, Kilian; Larese-Casanova, Philip Geochimica et Cosmochimica Acta, Vol. 81 https://doi.org/10.1016/j.gca.2011.12.014	journal	March 2012
Abiotic U(VI) reduction by aqueous sulfide Hyun, Sung Pil; Davis, James A.; Hayes, Kim F. Applied Geochemistry, Vol. 50 https://doi.org/10.1016/j.apgeochem.2014.07.021	journal	November 2014
Comparative Study of Uranyl(VI) and -(V) Carbonato Complexes in an Aqueous Solution Ikeda, Atsushi; Hennig, Christoph; Tsushima, Satoru Inorganic Chemistry, Vol. 46, Issue 10 https://doi.org/10.1021/ic070051y	journal	May 2007
Influence of Dynamical Conditions on the Reduction of U ^VI at the Magnetite−Solution Interface Ilton, Eugene S.; Boily, Jean-François; Buck, Edgar C. Environmental Science & Technology, Vol. 44, Issue 1 https://doi.org/10.1021/es9014597	journal	January 2010
Reduction of U(VI) Incorporated in the Structure of Hematite Ilton, Eugene S.; Pacheco, Juan S. Lezama; Bargar, John R. Environmental Science & Technology, Vol. 46, Issue 17 https://doi.org/10.1021/es3015502	journal	August 2012
Structural formula of uraninite Janeczek, J.; Ewing, R. C. Journal of Nuclear Materials, Vol. 190 https://doi.org/10.1016/0022-3115(92)90082-V	journal	August 1992
Fluorescence spectroscopy and microscopy as tools for monitoring redox transformations of uranium in biological systems Jones, Debbie L.; Andrews, Michael B.; Swinburne, Adam N. Chemical Science, Vol. 6, Issue 9 https://doi.org/10.1039/C5SC00661A	journal	January 2015
Atomistic Simulations of Uranium Incorporation into Iron (Hydr)Oxides Kerisit, Sebastien; Felmy, Andrew R.; Ilton, Eugene S. Environmental Science & Technology, Vol. 45, Issue 7 https://doi.org/10.1021/es1037639	journal	April 2011
Chemical State of Complex Uranium Oxides Kvashnina, K. O.; Butorin, S. M.; Martin, P. Physical Review Letters, Vol. 111, Issue 25 https://doi.org/10.1103/PhysRevLett.111.253002	journal	December 2013
Uranium(IV) remobilization under sulfate reducing conditions Lee, Seung Yeop; Cha, Wan Sik; Kim, Jong-Gu Chemical Geology, Vol. 370 https://doi.org/10.1016/j.chemgeo.2014.01.020	journal	March 2014
Local Structure in U(IV) and U(V) Environments: The Case of U ₃ O ₇ Leinders, Gregory; Bes, René; Kvashnina, Kristina O. Inorganic Chemistry, Vol. 59, Issue 7 https://doi.org/10.1021/acs.inorgchem.9b03702	journal	March 2020
X-ray absorption spectroscopy studies of reactions of technetium, uranium and neptunium with mackinawite Livens, Francis R.; Jones, Mark J.; Hynes, Amanda J. Journal of Environmental Radioactivity, Vol. 74, Issue 1-3 https://doi.org/10.1016/j.jenvrad.2004.01.012	journal	January 2004
Deep subsurface microbial processes Lovley, Derek R.; Chapelle, Francis H. Reviews of Geophysics, Vol. 33, Issue 3 https://doi.org/10.1029/95RG01305	journal	January 1995
Incorporation of Uranium into Hematite during Crystallization from Ferrihydrite Marshall, Timothy A.; Morris, Katherine; Law, Gareth T. W. Environmental Science & Technology, Vol. 48, Issue 7 https://doi.org/10.1021/es500212a	journal	March 2014
Uranium fate during crystallization of magnetite from ferrihydrite in conditions relevant to the disposal of radioactive waste Marshall, Timothy A.; Morris, Katherine; Law, Gareth T. W. Mineralogical Magazine, Vol. 79, Issue 6 https://doi.org/10.1180/minmag.2015.079.6.02	journal	November 2015
Trace Uranium Partitioning in a Multiphase Nano-FeOOH System McBriarty, Martin E.; Soltis, Jennifer A.; Kerisit, Sebastien Environmental Science & Technology, Vol. 51, Issue 9 https://doi.org/10.1021/acs.est.7b00432	journal	April 2017
Iron Vacancies Accommodate Uranyl Incorporation into Hematite McBriarty, Martin E.; Kerisit, Sebastien; Bylaska, Eric J. Environmental Science & Technology, Vol. 52, Issue 11 https://doi.org/10.1021/acs.est.8b00297	journal	May 2018
Uranium Uptake from Aqueous Solution by Interaction with Goethite, Lepidocrocite, Muscovite, and Mackinawite: An X-ray Absorption Spectroscopy Study Moyes, Lesley N.; Parkman, Richard H.; Charnock, John M. Environmental Science & Technology, Vol. 34, Issue 6 https://doi.org/10.1021/es990703k	journal	March 2000
The biogeochemistry and bioremediation of uranium and other priority radionuclides Newsome, Laura; Morris, Katherine; Lloyd, Jonathan R. Chemical Geology, Vol. 363 https://doi.org/10.1016/j.chemgeo.2013.10.034	journal	January 2014
Pyrite formation and mineral transformation pathways upon sulfidation of ferric hydroxides depend on mineral type and sulfide concentration Peiffer, Stefan; Behrends, Thilo; Hellige, Katrin Chemical Geology, Vol. 400 https://doi.org/10.1016/j.chemgeo.2015.01.023	journal	April 2015
Aqueous U(VI) interaction with magnetite nanoparticles in a mixed flow reactor system: HR-XANES study Pidchenko, I.; Heberling, F.; Kvashnina, Ko Journal of Physics: Conference Series, Vol. 712 https://doi.org/10.1088/1742-6596/712/1/012086	journal	May 2016
Uranium Redox Transformations after U(VI) Coprecipitation with Magnetite Nanoparticles Pidchenko, Ivan; Kvashnina, Kristina O.; Yokosawa, Tadahiro Environmental Science & Technology, Vol. 51, Issue 4 https://doi.org/10.1021/acs.est.6b04035	journal	February 2017
Further insights into the chemistry of the Bi–U–O system Popa, Karin; Prieur, Damien; Manara, Dario Dalton Transactions, Vol. 45, Issue 18 https://doi.org/10.1039/C6DT00735J	journal	January 2016
A revised scheme for the reactivity of iron (oxyhydr)oxide minerals towards dissolved sulfide Poulton, Simon W.; Krom, Michael D.; Raiswell, Robert Geochimica et Cosmochimica Acta, Vol. 68, Issue 18 https://doi.org/10.1016/j.gca.2004.03.012	journal	September 2004
ATHENA , ARTEMIS , HEPHAESTUS : data analysis for X-ray absorption spectroscopy using IFEFFIT Ravel, B.; Newville, M. Journal of Synchrotron Radiation, Vol. 12, Issue 4 https://doi.org/10.1107/S0909049505012719	journal	June 2005
Bioreduction of Uranium: Environmental Implications of a Pentavalent Intermediate Renshaw, Joanna C.; Butchins, Laura J. C.; Livens, Francis R. Environmental Science & Technology, Vol. 39, Issue 15 https://doi.org/10.1021/es048232b	journal	August 2005
Uranium(V) Incorporation Mechanisms and Stability in Fe(II)/Fe(III) (oxyhydr)Oxides Roberts, Hannah E.; Morris, Katherine; Law, Gareth T. W. Environmental Science & Technology Letters, Vol. 4, Issue 10 https://doi.org/10.1021/acs.estlett.7b00348	journal	September 2017
Fifteen Years of Radionuclide Research at the KIT Synchrotron Source in the Context of the Nuclear Waste Disposal Safety Case Rothe, Jörg; Altmaier, Marcus; Dagan, Ron Geosciences, Vol. 9, Issue 2 https://doi.org/10.3390/geosciences9020091	journal	February 2019
Complexation of uranium(VI) with protocatechuic acid?application of iterative transformation factor analysis to EXAFS spectroscopy Ro�berg, A.; Reich, T.; Bernhard, G. Analytical and Bioanalytical Chemistry, Vol. 376, Issue 5 https://doi.org/10.1007/s00216-003-1963-5	journal	July 2003
Surface complexation of U(VI) on goethite (α-FeOOH) Sherman, David M.; Peacock, Caroline L.; Hubbard, Christopher G. Geochimica et Cosmochimica Acta, Vol. 72, Issue 2 https://doi.org/10.1016/j.gca.2007.10.023	journal	January 2008
A multiplatform code for the analysis of energy-dispersive X-ray fluorescence spectra Solé, V. A.; Papillon, E.; Cotte, M. Spectrochimica Acta Part B: Atomic Spectroscopy, Vol. 62, Issue 1 https://doi.org/10.1016/j.sab.2006.12.002	journal	January 2007
Abiotic Reductive Immobilization of U(VI) by Biogenic Mackinawite Veeramani, Harish; Scheinost, Andreas C.; Monsegue, Niven Environmental Science & Technology, Vol. 47, Issue 5 https://doi.org/10.1021/es304025x	journal	February 2013
Multiple Lines of Evidence Identify U(V) as a Key Intermediate during U(VI) Reduction by Shewanella oneidensis MR1 Vettese, Gianni F.; Morris, Katherine; Natrajan, Louise S. Environmental Science & Technology, Vol. 54, Issue 4 https://doi.org/10.1021/acs.est.9b05285	journal	January 2020
The role of the 5f valence orbitals of early actinides in chemical bonding Vitova, T.; Pidchenko, I.; Fellhauer, D. Nature Communications, Vol. 8, Issue 1 https://doi.org/10.1038/ncomms16053	journal	July 2017
Competitive Reaction of Neptunium(V) and Uranium(VI) in Potassium–Sodium Carbonate-Rich Aqueous Media: Speciation Study with a Focus on High-Resolution X-ray Spectroscopy Vitova, Tonya; Pidchenko, Ivan; Schild, Dieter Inorganic Chemistry, Vol. 59, Issue 1 https://doi.org/10.1021/acs.inorgchem.9b02463	journal	December 2019
Uranium(VI) adsorption to ferrihydrite: Application of a surface complexation model Waite, T. D.; Davis, J. A.; Payne, T. E. Geochimica et Cosmochimica Acta, Vol. 58, Issue 24 https://doi.org/10.1016/0016-7037(94)90243-7	journal	December 1994
Occurrence of Surface Polysulfides during the Interaction between Ferric (Hydr)Oxides and Aqueous Sulfide Wan, Moli; Shchukarev, Andrey; Lohmayer, Regina Environmental Science & Technology, Vol. 48, Issue 9 https://doi.org/10.1021/es405612f	journal	April 2014
Fe(III):S(-II) concentration ratio controls the pathway and the kinetics of pyrite formation during sulfidation of ferric hydroxides Wan, Moli; Schröder, Christian; Peiffer, Stefan Geochimica et Cosmochimica Acta, Vol. 217 https://doi.org/10.1016/j.gca.2017.08.036	journal	November 2017
Ferrihydrite Formation: The Role of Fe ₁₃ Keggin Clusters Weatherill, Joshua S.; Morris, Katherine; Bots, Pieter Environmental Science & Technology, Vol. 50, Issue 17 https://doi.org/10.1021/acs.est.6b02481	journal	August 2016
U(VI) sorption during ferrihydrite formation: Underpinning radioactive effluent treatment Winstanley, Ellen H.; Morris, Katherine; Abrahamsen-Mills, Liam G. Journal of Hazardous Materials, Vol. 366 https://doi.org/10.1016/j.jhazmat.2018.11.077	journal	March 2019
The CAT-ACT Beamline at ANKA: A new high energy X-ray spectroscopy facility for CATalysis and ACTinide research Zimina, A.; Dardenne, K.; Denecke, M. A. Journal of Physics: Conference Series, Vol. 712 https://doi.org/10.1088/1742-6596/712/1/012019	journal	May 2016
CAT-ACT—A new highly versatile x-ray spectroscopy beamline for catalysis and radionuclide science at the KIT synchrotron light facility ANKA Zimina, A.; Dardenne, K.; Denecke, M. A. Review of Scientific Instruments, Vol. 88, Issue 11 https://doi.org/10.1063/1.4999928	journal	November 2017

Similar Records

Trace Uranium Partitioning in a Multiphase Nano-FeOOH System

Journal Article · 2017 · Environmental Science and Technology · OSTI ID:1355047

McBriarty, Martin E.; Soltis, Jennifer A.; Kerisit, Sebastien; +5 more

Sulfidation of magnetite with incorporated uranium

Citation Formats

References (67)

Similar Records

Related Subjects