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Title: MESOSCALE BIOTRANSFORMATIONS OF URANIUM IN SEDIMENTS AND SOILS (Program Element: Biogeochemistry)

Abstract

In-situ bioreduction is being considered as a remediation strategy for uranium (U) contaminated sediments because of its potentially low cost, and because short-term studies support its feasibility. However, any in-situ approach for immobilizing U will require assurance of either permanent fixation, or of very low release rates into the biosphere. Our long-term laboratory studies have shown that reoxidation of bioreduced UO{sub 2} can occur even under reducing (methanogenic) conditions sustained by continuous infusion of lactate. The biogeochemical processes underlying this finding need to be understood. Our current research is designed to identify mechanisms responsible for anaerobic U oxidation, and identify effects of key factors controlling long-term stability of bioreduced U. These include: (1) effects of organic carbon (OC) concentrations and supply rates on stability of bioreduced U, (2) influences of pH on U(IV)/U(VI) redox equilibrium, (3) the roles of Fe- and Mn-oxides as potential U oxidants in sediments, and (4) the role of microorganisms in U reoxidation. Findings from some of these studies are summarized here.

Authors:
; ; ; ; ; ; ; ; ;
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA; University of California, Berkeley, CA; University of Chicago, Chicago, IL; University of Georgia, Athens, GA
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
894504
Report Number(s):
CONF-ERSP2006-29
TRN: US0700178
Resource Type:
Conference
Resource Relation:
Conference: Annual Environmental Remediation Sciences Program PI Meeting, April 3-5, 2006, Warrenton, VA
Country of Publication:
United States
Language:
English
Subject:
38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY; 54 ENVIRONMENTAL SCIENCES; 59 BASIC BIOLOGICAL SCIENCES; AVAILABILITY; BIOGEOCHEMISTRY; BIOSPHERE; CARBON; INFUSION; MICROORGANISMS; OXIDATION; OXIDIZERS; SEDIMENTS; SOILS; STABILITY; URANIUM

Citation Formats

Tetsu Tokunaga, Jiamin Wan, Brodic, Eoin, Yongman Kim, Hazen, Terry, Firestone, Mary, Herman, Don, Sutton, Steve, Newville, Matt, and Lanzirotti, Tony, Rao, Bill. MESOSCALE BIOTRANSFORMATIONS OF URANIUM IN SEDIMENTS AND SOILS (Program Element: Biogeochemistry). United States: N. p., 2006. Web.
Tetsu Tokunaga, Jiamin Wan, Brodic, Eoin, Yongman Kim, Hazen, Terry, Firestone, Mary, Herman, Don, Sutton, Steve, Newville, Matt, & Lanzirotti, Tony, Rao, Bill. MESOSCALE BIOTRANSFORMATIONS OF URANIUM IN SEDIMENTS AND SOILS (Program Element: Biogeochemistry). United States.
Tetsu Tokunaga, Jiamin Wan, Brodic, Eoin, Yongman Kim, Hazen, Terry, Firestone, Mary, Herman, Don, Sutton, Steve, Newville, Matt, and Lanzirotti, Tony, Rao, Bill. Wed . "MESOSCALE BIOTRANSFORMATIONS OF URANIUM IN SEDIMENTS AND SOILS (Program Element: Biogeochemistry)". United States. doi:. https://www.osti.gov/servlets/purl/894504.
@article{osti_894504,
title = {MESOSCALE BIOTRANSFORMATIONS OF URANIUM IN SEDIMENTS AND SOILS (Program Element: Biogeochemistry)},
author = {Tetsu Tokunaga and Jiamin Wan and Brodic, Eoin and Yongman Kim and Hazen, Terry and Firestone, Mary and Herman, Don and Sutton, Steve and Newville, Matt and Lanzirotti, Tony, Rao, Bill},
abstractNote = {In-situ bioreduction is being considered as a remediation strategy for uranium (U) contaminated sediments because of its potentially low cost, and because short-term studies support its feasibility. However, any in-situ approach for immobilizing U will require assurance of either permanent fixation, or of very low release rates into the biosphere. Our long-term laboratory studies have shown that reoxidation of bioreduced UO{sub 2} can occur even under reducing (methanogenic) conditions sustained by continuous infusion of lactate. The biogeochemical processes underlying this finding need to be understood. Our current research is designed to identify mechanisms responsible for anaerobic U oxidation, and identify effects of key factors controlling long-term stability of bioreduced U. These include: (1) effects of organic carbon (OC) concentrations and supply rates on stability of bioreduced U, (2) influences of pH on U(IV)/U(VI) redox equilibrium, (3) the roles of Fe- and Mn-oxides as potential U oxidants in sediments, and (4) the role of microorganisms in U reoxidation. Findings from some of these studies are summarized here.},
doi = {},
journal = {},
number = ,
volume = ,
place = {United States},
year = {Wed Apr 05 00:00:00 EDT 2006},
month = {Wed Apr 05 00:00:00 EDT 2006}
}

Conference:
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  • Bioreduction of U in contaminated sediments is an attractive strategy because of its low cost, and because of short-term studies supporting its feasibility. However, any in-situ immobilization approach for U will require assurance of either permanent fixation, or of very low release rates into the biosphere. Our previous long-term (2 years) laboratory experiments have shown that organic carbon (OC) based U(VI) bioreduction to UO2 can be transient even under sustained reducing (methanogenic) conditions. The biogeochemical processes underlying this finding urgently need to be understood. The current research is designed to identify mechanisms responsible for anaerobic U oxidation, and identify conditionsmore » that will support long-term stability of bioreduced U. We are investigating: (1) effects of OC concentration and supply rate on remobilization of bioreduced U, (2) the roles of Fe- and Mn-oxides as potential U oxidants in sediments, and (3) the role of microorganisms in U reoxidation, and (4) influences of pH on U(IV)/U(VI) redox equilibrium.« less
  • An integrated approach to remove uranium from uranium-contaminated soils is being conducted by four of the US Department of Energy national laboratories. In this approach, managed through the Uranium in Soils Integrated Demonstration program at the Fernald Environmental Management Project, Fernald, Ohio, these laboratories are developing processes that selectively remove uranium from soil without seriously degrading the soil`s physicochemical characteristics or generating waste that is difficult to manage or dispose of. These processes include traditional uranium extractions that use carbonate as well as some nontraditional extraction techniques that use citric acid and complex organic chelating agents such as naturally occurringmore » microbial siderophores. A bench-scale engineering design for heap leaching; a process that uses carbonate leaching media shows that >90% of the uranium can be removed from the Fernald soils. Other work involves amending soils with cultures of sulfur and ferrous oxidizing microbes or cultures of fungi whose role is to generate mycorrhiza that excrete strong complexers for uranium. Aqueous biphasic extraction, a physical separation technology, is also being evaluated because of its ability to segregate fine particulate, a fundamental requirement for soils containing high levels of silt and clay. Interactions among participating scientists have produced some significant progress not only in evaluating the feasibility of uranium removal but also in understanding some important technical aspects of the task.« less
  • DOE sites are contaminated by radionuclides and toxic metals, which are in contact with organic contaminants, reactive minerals, and diverse populations of microorganisms. Actinide species to be stabilized or mobilized in situ via direct and indirect chemical, biological, and geochemical processes. Actinide contamination tends to be broadly dispersed and present at low concentrations and therefore prohibitively costly to remove using conventional methods. Pu contamination is particularly challenging because of personnel exposure concerns and a lack of disposal sites. Bacterial bioremediation is a preferable treatment approach. Given that the radionuclides of most concern to the NABIR program are generally more mobilemore » in their oxidized forms (e.g. Pu(VI), Pu(V), U(VI), Tc(VII), Cr(VI)), proposed biostabilization strategies are generally based upon either in situ sequestration of the oxidized form (e.g. actinide biosorption and bioaccumulation within exopolymers and biofilms) or biomineralization of the reduced form (e.g., direct or indirect production of insoluble hydroxides by DMRB). The feasibility of these approaches is affected by the speciation of actinides under environment conditions. For example, actinides can form complexes with co-contaminants (e.g. EDTA) or natural chelators like siderophores and biopolymers. Resulting complexes can interact with bacteria in several ways to yield biostabilized products or more mobile species that could persist. They are investigating how organic chelators affect the speciation and biotransformation of U and Pu. Previously, they reported how these siderophores bind, desorb and solubilize radionuclides. Here they present new results on EDTA complexation, siderophore-mediated Pu accumulation by aerobic bacteria, and initial studies of Pu reduction by DMRB.« less
  • The responses of the continental slope benthos to organic detritus deposition were studied with a multiple trace approach. Study sites were offshore of Cape Fear (I) and Cape Hatteras (III), N.C. (both 850 m water depth) and were characterized by different organic C deposition rates, macrofaunal densities (III>I in both cases) and taxa. Natural abundances of {sup 13}C and {sup 12}C in particulate organic carbon (POC), dissolved inorganic carbon (DIC) and macrofauna indicate that the reactive organic detritus is marine in origin. Natural abundance levels of {sup 14}C and uptake of {sup 13}C-labeled diatoms by benthic animals indicate that theymore » incorporate a relatively young component of carbon into their biomass. {sup 13}C-labeled diatoms (Thalassiorsira pseudonana) tagged with {sup 210}Pb, slope sediment tagged with {sup 113}Sn and {sup 228}Th-labeled glass beads were emplaced in plots on the seafloor at both locations and the plots were sampled after 30 min., 1-1.5 d and 14 mo. At Site I, tracer diatom was intercepted at the surface primarily by protozoans and surface-feeding annelids. Little of the diatom C penetrated below 2 cm even after 14 months. Oxidation of organic carbon appeared to be largely aerobic. At Site III, annelids were primarily responsible for the initial uptake of tracer. On the time scale of days, diatom C was transported to a depth of 12 cm and was found in animals collected between 5-10 cm. The hoeing of tracer from the surface by the maldanid Praxillela sp. may have been responsible for some of the rapid nonlocal transport. Oxidation of the diatom organic carbon was evident to at least 10 cm depth. Anaerobic breakdown of organic matter is more important at Site III. Horizontal transport, which was probably biologically mediated, was an order of magnitude more rapid than vertical displacement over a year time scale. If the horizontal transport was associated with biochemical transformations of the organic matter, it may represent an important but nearly invisible diagenetic process.« less