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Title: Complexation by Organic Matter Controls Uranium Mobility in Anoxic Sediments

Journal Article · · Environmental Science and Technology

Uranium contamination threatens the availability of safe and clean drinking water globally. This toxic element occurs both naturally and as a result of mining and ore-processing in alluvial sediments, where it accumulates as tetravalent U [U(IV)], a form once considered largely immobile. Changing hydrologic and geochemical conditions cause U to be released into groundwater. Knowledge of the chemical form(s) of U(IV) is essential to understand the release mechanism, however, the relevant U(IV) species are poorly characterized. There is growing belief that natural organic matter (OM) binds U(IV) and mediates its fate in the subsurface. In this work, we combined nanoscale imaging (nano secondary ion mass spectrometry and scanning transmission X-ray microscopy) with a density-based fractionation approach to physically and microscopically isolate organic and mineral matter from alluvial sediments contaminated with uranium. We identified two populations of U (dominantly +IV) in anoxic sediments. Uranium was retained on OM and adsorbed to particulate organic carbon, comprising both microbial and plant material. Surprisingly, U was also adsorbed to clay minerals and OM-coated clay minerals. The dominance of OM-associated U provides a framework to understand U mobility in the shallow subsurface, and, in particular, emphasizes roles for desorption and colloid formation in its mobilization.

Research Organization:
SLAC National Accelerator Lab., Menlo Park, CA (United States); Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL)
Sponsoring Organization:
USDOE Office of Science (SC), Biological and Environmental Research (BER); Natural Sciences and Engineering Research Council of Canada (NSERC); Canadian Institutes of Health Research (CIHR); National Research Council Canada (NRC); Western Economic Diversification Canada; Province of Saskatchewan
Grant/Contract Number:
AC02-76SF00515; AC05-76RL01830
OSTI ID:
1605282
Alternate ID(s):
OSTI ID: 1600519
Report Number(s):
PNNL-SA-142857; TRN: US2104413
Journal Information:
Environmental Science and Technology, Vol. 54, Issue 3; ISSN 0013-936X
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 21 works
Citation information provided by
Web of Science

References (51)

Natural Uranium Contamination in Major U.S. Aquifers Linked to Nitrate journal July 2015
National trends in drinking water quality violations journal February 2018
Large-Scale Uranium Contamination of Groundwater Resources in India journal May 2018
Effects of Groundwater Development on Uranium: Central Valley, California, USA journal November 2010
Physico-Chemical Heterogeneity of Organic-Rich Sediments in the Rifle Aquifer, CO: Impact on Uranium Biogeochemistry journal December 2015
Persistence of uranium groundwater plumes: Contrasting mechanisms at two DOE sites in the groundwater–river interaction zone journal April 2013
Refining the site conceptual model at a former uranium mill site in Riverton, Wyoming, USA journal July 2015
Redox Controls over the Stability of U(IV) in Floodplains of the Upper Colorado River Basin journal September 2017
Quantitative Separation of Monomeric U(IV) from UO 2 in Products of U(VI) Reduction journal May 2012
Relative Reactivity of Biogenic and Chemogenic Uraninite and Biogenic Noncrystalline U(IV) journal August 2013
Uranium(IV) adsorption by natural organic matter in anoxic sediments journal January 2017
Non-uraninite Products of Microbial U(VI) Reduction journal December 2010
Mechanism of Uranium Reduction and Immobilization in Desulfovibrio vulgaris Biofilms journal August 2015
The product of microbial uranium reduction includes multiple species with U(IV)–phosphate coordination journal April 2014
Molecular Structure in Soil Humic Substances:  The New View journal December 2005
Geochemical, mineralogical and microbiological characteristics of sediment from a naturally reduced zone in a uranium-contaminated aquifer journal August 2012
Uranium redox transition pathways in acetate-amended sediments journal March 2013
Density fractions versus size separates: does physical fractionation isolate functional soil compartments? journal January 2012
Anaerobic microsites have an unaccounted role in soil carbon stabilization journal November 2017
Mineral protection of soil carbon counteracted by root exudates journal March 2015
Calcium-mediated stabilisation of soil organic carbon journal December 2017
Understanding controls on redox processes in floodplain sediments of the Upper Colorado River Basin journal December 2017
Carbon (1s) NEXAFS Spectroscopy of Biogeochemically Relevant Reference Organic Compounds journal January 2009
Microscopic characterization of carbonaceous aerosol particle aging in the outflow from Mexico City journal January 2010
Quantitative mapping of chlorhexidine in natural river biofilms journal October 2006
Cluster analysis of soft X-ray spectromicroscopy data journal July 2004
Distribution of hydrous aluminium and iron over density fractions depends on organic matter load and ultrasonic dispersion journal June 2007
Clay-sized organo-mineral complexes in a cultivation chronosequence: revisiting the concept of the 'primary organo-mineral complex' journal August 2006
Spectroscopic Evidence of Uranium Immobilization in Acidic Wetlands by Natural Organic Matter and Plant Roots journal February 2015
Tetra- and Hexavalent Uranium Forms Bidentate-Mononuclear Complexes with Particulate Organic Matter in a Naturally Uranium-Enriched Peatland journal September 2016
Oxidative Uranium Release from Anoxic Sediments under Diffusion-Limited Conditions journal September 2017
Mobile uranium(IV)-bearing colloids in a mining-impacted wetland journal December 2013
Biogenic non-crystalline U(IV) revealed as major component in uranium ore deposits journal June 2017
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 journal August 2006
Long-Term in Situ Oxidation of Biogenic Uraninite in an Alluvial Aquifer: Impact of Dissolved Oxygen and Calcium journal June 2015
Introduction of Soft X-Ray Spectromicroscopy as an Advanced Technique for Plant Biopolymers Research journal March 2015
Organic carbon distribution, speciation, and elemental correlations within soil microaggregates: Applications of STXM and NEXAFS spectroscopy journal November 2007
Nano-scale investigation of the association of microbial nitrogen residues with iron (hydr)oxides in a forest soil O-horizon journal October 2012
STXM and NanoSIMS Investigations on EPS Fractions before and after Adsorption to Goethite journal March 2013
Micro- and nano-environments of carbon sequestration: Multi-element STXM–NEXAFS spectromicroscopy assessment of microbial carbon and mineral associations journal November 2012
Iron and Carbon Dynamics during Aging and Reductive Transformation of Biogenic Ferrihydrite journal December 2015
Redox Interactions of Tc(VII), U(VI), and Np(V) with Microbially Reduced Biotite and Chlorite journal November 2015
Uranium Reduction by Fe(II) in the Presence of Montmorillonite and Nontronite journal July 2016
Modeling uranium(VI) adsorption onto montmorillonite under varying carbonate concentrations: A surface complexation model accounting for the spillover effect on surface potential journal January 2018
Uranium(VI) adsorption and surface complexation modeling onto vadose sediments from the Savannah River Site journal February 2018
Partitioning of uranyl between ferrihydrite and humic substances at acidic and circum-neutral pH journal October 2017
Acetate Availability and its Influence on Sustainable Bioremediation of Uranium-Contaminated Groundwater journal June 2011
Mononuclear U(IV) complexes and ningyoite as major uranium species in lake sediments journal January 2016
Uranium Retention in a Bioreduced Region of an Alluvial Aquifer Induced by the Influx of Dissolved Oxygen journal June 2018
Colloid Mobilization During Soil Iron Redox Oscillations journal September 2006
Mobilization of colloidal carbon during iron reduction in basaltic soils journal June 2014

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