Uranium(IV) adsorption by natural organic matter in anoxic sediments

Bone, Sharon E.; Dynes, James J.; Cliff, John; Bargar, John R.

doi:10.1073/pnas.1611918114

Title: Uranium(IV) adsorption by natural organic matter in anoxic sediments

Journal Article · 08 January 2017 · Proceedings of the National Academy of Sciences of the United States of America

DOI: https://doi.org/10.1073/pnas.1611918114 · OSTI ID:1338629

Bone, Sharon E. ^[1]; Dynes, James J. ^[2]; Cliff, John ^[3]; Bargar, John R. ^[1]

Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, Menlo Park, CA 94025,
Canadian Light Source, Saskatoon, SK S7N 2V3, Canada,
Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland, WA 99354

Significance Uranium is an important fuel source and pollutant, and its chemical form determines its reactivity in the environment. However, information on the speciation of tetravalent U [U(IV)] in sediments is lacking. The research presented herein takes a holistic view of U(IV) speciation in a natural material containing microbial cells, organic matter, and minerals. Our work demonstrates unequivocally that U(IV) adsorbs to natural organic matter under anoxic, field-relevant conditions. Furthermore, we put forward a conceptual model that provides a framework for future studies of U biogeochemistry in which postreduction surface complexation processes can be used to predict U(IV) behavior. Our work has ramifications for remediation of U-contaminated sites and also informs in situ mining practices.

View Journal Article

Cite

Export

Save

Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States), Environmental Molecular Sciences Laboratory (EMSL); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23)

Grant/Contract Number:: AC02-76SF00515; AC05-76RL01830

OSTI ID:: 1338629

Report Number(s):: PNNL-SA--119314; SLAC-PUB--16909

Journal Information:: Proceedings of the National Academy of Sciences of the United States of America, Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Issue: 4 Vol. 114; ISSN 0027-8424

Publisher:: Proceedings of the National Academy of SciencesCopyright Statement

Country of Publication:: United States

Language:: English

References (45)

Actinides in Solution: Complexation and Kinetics Choppin, Gregory R.; Jensen, Mark P. The Chemistry of the Actinide and Transactinide Elements https://doi.org/10.1007/1-4020-3598-5_23	book	January 2007
Influence of hydrological, biogeochemical and temperature transients on subsurface carbon fluxes in a flood plain environment Arora, Bhavna; Spycher, Nicolas F.; Steefel, Carl I. Biogeochemistry, Vol. 127, Issue 2-3 https://doi.org/10.1007/s10533-016-0186-8	journal	February 2016
Geochemical, mineralogical and microbiological characteristics of sediment from a naturally reduced zone in a uranium-contaminated aquifer Campbell, K. M.; Kukkadapu, R. K.; Qafoku, N. P. Applied Geochemistry, Vol. 27, Issue 8 https://doi.org/10.1016/j.apgeochem.2012.04.013	journal	August 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
Biogeochemical aspects of uranium mineralization, mining, milling, and remediation Campbell, Kate M.; Gallegos, Tanya J.; Landa, Edward R. Applied Geochemistry, Vol. 57 https://doi.org/10.1016/j.apgeochem.2014.07.022	journal	June 2015
Competition between enzymatic and abiotic reduction of uranium(VI) under iron reducing conditions Behrends, Thilo; Van Cappellen, Philippe Chemical Geology, Vol. 220, Issue 3-4 https://doi.org/10.1016/j.chemgeo.2005.04.007	journal	August 2005
Characterization of cores from an in-situ recovery mined uranium deposit in Wyoming: Implications for post-mining restoration WoldeGabriel, G.; Boukhalfa, H.; Ware, S. D. Chemical Geology, Vol. 390 https://doi.org/10.1016/j.chemgeo.2014.10.009	journal	December 2014
Chemical composition of the graphitic black carbon fraction in riverine and marine sediments at sub-micron scales using carbon X-ray spectromicroscopy Haberstroh, Paul R.; Brandes, Jay A.; Gélinas, Yves Geochimica et Cosmochimica Acta, Vol. 70, Issue 6 https://doi.org/10.1016/j.gca.2005.12.001	journal	March 2006
Organic carbon distribution, speciation, and elemental correlations within soil microaggregates: Applications of STXM and NEXAFS spectroscopy Wan, Jiamin; Tyliszczak, Tolek; Tokunaga, Tetsu K. Geochimica et Cosmochimica Acta, Vol. 71, Issue 22 https://doi.org/10.1016/j.gca.2007.07.030	journal	November 2007
Products of abiotic U(VI) reduction by biogenic magnetite and vivianite Veeramani, Harish; Alessi, Daniel S.; Suvorova, Elena I. Geochimica et Cosmochimica Acta, Vol. 75, Issue 9 https://doi.org/10.1016/j.gca.2011.02.024	journal	May 2011
Uranium speciation and stability after reductive immobilization in aquifer sediments Sharp, Jonathan O.; Lezama-Pacheco, Juan S.; Schofield, Eleanor J. Geochimica et Cosmochimica Acta, Vol. 75, Issue 21 https://doi.org/10.1016/j.gca.2011.08.022	journal	November 2011
Nano-scale investigation of the association of microbial nitrogen residues with iron (hydr)oxides in a forest soil O-horizon Keiluweit, Marco; Bougoure, Jeremy J.; Zeglin, Lydia H. Geochimica et Cosmochimica Acta, Vol. 95 https://doi.org/10.1016/j.gca.2012.07.001	journal	October 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
Isotope fractionation during oxidation of tetravalent uranium by dissolved oxygen Wang, Xiangli; Johnson, Thomas M.; Lundstrom, Craig C. Geochimica et Cosmochimica Acta, Vol. 150 https://doi.org/10.1016/j.gca.2014.12.007	journal	February 2015
Uranium removal from groundwater via in situ biostimulation: Field-scale modeling of transport and biological processes Yabusaki, Steven B.; Fang, Yilin; Long, Philip E. Journal of Contaminant Hydrology, Vol. 93, Issue 1-4 https://doi.org/10.1016/j.jconhyd.2007.02.005	journal	August 2007
Variably saturated flow and multicomponent biogeochemical reactive transport modeling of a uranium bioremediation field experiment Yabusaki, Steven B.; Fang, Yilin; Williams, Kenneth H. Journal of Contaminant Hydrology, Vol. 126, Issue 3-4 https://doi.org/10.1016/j.jconhyd.2011.09.002	journal	November 2011
Quantitative mapping of chlorhexidine in natural river biofilms Dynes, James J.; Lawrence, John R.; Korber, Darren R. Science of The Total Environment, Vol. 369, Issue 1-3 https://doi.org/10.1016/j.scitotenv.2006.04.033	journal	October 2006
Cluster analysis of soft X-ray spectromicroscopy data Lerotic, M.; Jacobsen, C.; Schäfer, T. Ultramicroscopy, Vol. 100, Issue 1-2 https://doi.org/10.1016/j.ultramic.2004.01.008	journal	July 2004
Mechanism of Uranium Reduction and Immobilization in Desulfovibrio vulgaris Biofilms Stylo, Malgorzata; Neubert, Nadja; Roebbert, Yvonne Environmental Science & Technology, Vol. 49, Issue 17 https://doi.org/10.1021/acs.est.5b01769	journal	August 2015
Physico-Chemical Heterogeneity of Organic-Rich Sediments in the Rifle Aquifer, CO: Impact on Uranium Biogeochemistry Janot, Noémie; Lezama Pacheco, Juan S.; Pham, Don Q. Environmental Science & Technology, Vol. 50, Issue 1 https://doi.org/10.1021/acs.est.5b03208	journal	December 2015
Tetra- and Hexavalent Uranium Forms Bidentate-Mononuclear Complexes with Particulate Organic Matter in a Naturally Uranium-Enriched Peatland Mikutta, Christian; Langner, Peggy; Bargar, John R. Environmental Science & Technology, Vol. 50, Issue 19 https://doi.org/10.1021/acs.est.6b03688	journal	September 2016
Measurement and Modeling of U(IV) Adsorption to Metal Oxide Minerals Wang, Zimeng; Ulrich, Kai-Uwe; Pan, Chao Environmental Science & Technology Letters, Vol. 2, Issue 8 https://doi.org/10.1021/acs.estlett.5b00156	journal	July 2015
Determination of the Formation Constants of Ternary Complexes of Uranyl and Carbonate with Alkaline Earth Metals (Mg ²⁺ , Ca ²⁺ , Sr ²⁺ , and Ba ²⁺ ) Using Anion Exchange Method Dong, Wenming; Brooks, Scott C. Environmental Science & Technology, Vol. 40, Issue 15 https://doi.org/10.1021/es0606327	journal	August 2006
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
Solution and Microbial Controls on the Formation of Reduced U(IV) Species Boyanov, Maxim I.; Fletcher, Kelly E.; Kwon, Man Jae Environmental Science & Technology, Vol. 45, Issue 19 https://doi.org/10.1021/es2014049	journal	October 2011
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
STXM and NanoSIMS Investigations on EPS Fractions before and after Adsorption to Goethite Liu, Xinran; Eusterhues, Karin; Thieme, Jürgen Environmental Science & Technology, Vol. 47, Issue 7 https://doi.org/10.1021/es3039505	journal	March 2013
Adsorption of Uranium(VI) to Manganese Oxides: X-ray Absorption Spectroscopy and Surface Complexation Modeling Wang, Zimeng; Lee, Sung-Woo; Catalano, Jeffrey G. Environmental Science & Technology, Vol. 47, Issue 2 https://doi.org/10.1021/es304454g	journal	December 2012
Bioreduction of Hydrogen Uranyl Phosphate: Mechanisms and U(IV) Products Rui, Xue; Kwon, Man Jae; O’Loughlin, Edward J. Environmental Science & Technology, Vol. 47, Issue 11 https://doi.org/10.1021/es305258p	journal	May 2013
Relative Reactivity of Biogenic and Chemogenic Uraninite and Biogenic Noncrystalline U(IV) Cerrato, José M.; Ashner, Matthew N.; Alessi, Daniel S. Environmental Science & Technology, Vol. 47, Issue 17 https://doi.org/10.1021/es401663t	journal	August 2013
Biogeochemical Controls on the Product of Microbial U(VI) Reduction Stylo, Malgorzata; Alessi, Daniel S.; Shao, Paul PaoYun Environmental Science & Technology, Vol. 47, Issue 21 https://doi.org/10.1021/es402631w	journal	October 2013
Stable U(IV) Complexes Form at High-Affinity Mineral Surface Sites Latta, Drew E.; Mishra, Bhoopesh; Cook, Russell E. Environmental Science & Technology, Vol. 48, Issue 3 https://doi.org/10.1021/es4047389	journal	January 2014
Thermodynamic Controls on the Microbial Reduction of Iron-Bearing Nontronite and Uranium Luan, Fubo; Gorski, Christopher A.; Burgos, William D. Environmental Science & Technology, Vol. 48, Issue 5 https://doi.org/10.1021/es404885e	journal	February 2014
Speciation and Reactivity of Uranium Products Formed during in Situ Bioremediation in a Shallow Alluvial Aquifer Alessi, Daniel S.; Lezama-Pacheco, Juan S.; Janot, Noémie Environmental Science & Technology, Vol. 48, Issue 21 https://doi.org/10.1021/es502701u	journal	October 2014
Validating the Scalability of Soft X-ray Spectromicroscopy for Quantitative Soil Ecology and Biogeochemistry Research Dynes, James J.; Regier, Tom Z.; Snape, Ian Environmental Science & Technology, Vol. 49, Issue 2 https://doi.org/10.1021/es505271p	journal	January 2015
Structure of Biogenic Uraninite Produced by Shewanella oneidensis Strain MR-1 Schofield, Eleanor J.; Veeramani, Harish; Sharp, Jonathan O. Environmental Science & Technology, Vol. 42, Issue 21 https://doi.org/10.1021/es800579g	journal	November 2008
Rapid expansion of oceanic anoxia immediately before the end-Permian mass extinction Brennecka, G. A.; Herrmann, A. D.; Algeo, T. J. Proceedings of the National Academy of Sciences, Vol. 108, Issue 43 https://doi.org/10.1073/pnas.1106039108	journal	October 2011
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
Acetate Availability and its Influence on Sustainable Bioremediation of Uranium-Contaminated Groundwater Williams, Kenneth H.; Long, Philip E.; Davis, James A. Geomicrobiology Journal, Vol. 28, Issue 5-6 https://doi.org/10.1080/01490451.2010.520074	journal	June 2011
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
Beam-induced oxidation of monomeric U(IV) species Alessi, Daniel S.; Uster, Benjamin; Borca, Camelia N. Journal of Synchrotron Radiation, Vol. 20, Issue 1 https://doi.org/10.1107/S0909049512041763	journal	November 2012
Organic chemical differentiation within fossil plant cell walls detected with X-ray spectromicroscopy Kevin Boyce, C.; Cody, George D.; Feser, Michael Geology, Vol. 30, Issue 11 https://doi.org/10.1130/0091-7613(2002)030<1039:OCDWFP>2.0.CO;2	journal	January 2002
Nanoscale Biogeocomplexity of the Organomineral Assemblage in Soil Kinyangi, James; Solomon, Dawit; Liang, Biqing Soil Science Society of America Journal, Vol. 70, Issue 5 https://doi.org/10.2136/sssaj2005.0351	journal	January 2006
Carbon (1s) NEXAFS Spectroscopy of Biogeochemically Relevant Reference Organic Compounds Solomon, Dawit; Lehmann, Johannes; Kinyangi, James Soil Science Society of America Journal, Vol. 73, Issue 6 https://doi.org/10.2136/sssaj2008.0228	journal	January 2009
Microscopic characterization of carbonaceous aerosol particle aging in the outflow from Mexico City Moffet, R. C.; Henn, T. R.; Tivanski, A. V. Atmospheric Chemistry and Physics, Vol. 10, Issue 3 https://doi.org/10.5194/acp-10-961-2010	journal	January 2010

Similar Records

Complexation by Organic Matter Controls Uranium Mobility in Anoxic Sediments

Journal Article · 2019 · Environmental Science and Technology · OSTI ID:1600519

Bone, Sharon E.; Cliff, John; Weaver, Karrie; +4 more

Carbonate Facilitated Mobilization of Uranium from Lacustrine Sediments under Anoxic Conditions

Journal Article · 2018 · Environmental Science and Technology · OSTI ID:1476326

Seder-Colomina, Marina; Mangeret, Arnaud; Stetten, Lucie; +8 more

Diagenetic formation of uranium-silica polymers in lake sediments over 3,300 years

Journal Article · 2021 · Proceedings of the National Academy of Sciences of the United States of America · OSTI ID:1761269

Lefebvre, Pierre; Gourgiotis, Alkiviadis; Mangeret, Arnaud; +16 more

Related Subjects

36 MATERIALS SCIENCE
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
58 GEOSCIENCES
EARTH
ENV
Environmental Molecular Sciences Laboratory

Title: Uranium(IV) adsorption by natural organic matter in anoxic sediments

Citation Formats

References (45)

Similar Records

Related Subjects