skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Investigation of Technetium Redox Cycling in FRC Background Sediments using EXAFS and Gamma Camera Imaging

Abstract

Technetium-99 is a priority pollutant at numerous DOE sites, due to its long half-life (2.1 x 105 years), high mobility as Tc(VII) in oxic waters, and bioavailability as a sulfate analogue. {sup 99}Tc is far less mobile under anaerobic conditions, forming insoluble Tc(IV) precipitates. As anaerobic microorganisms can reduce soluble Tc(VII) to insoluble Tc(IV), microbial metabolism may have the potential to treat sediments and waters contaminated with Tc. Baseline studies of fundamental mechanisms of Tc(VII) bioreduction and precipitation (reviewed by Lloyd et al., 2005, in press) have generally used pure cultures of metal-reducing bacteria, in order to develop conceptual models for the biogeochemical cycling of {sup 99}Tc. There is, however, comparatively little known about interactions of metal-reducing bacteria with environmentally relevant trace concentrations of {sup 99}Tc, against a more complex biogeochemical background provided by mixed microbial communities in aquifer sediments. The objective of this project is to probe the site specific biogeochemical conditions that control the mobility of {sup 99}Tc at the US DOE Field Research Center Site (FRC; Oak Ridge, Tennessee). This information is required for the rational design of in situ bioremediation strategies for technetium-contaminated subsurface environments. We are using a combination of geochemical, mineralogical, microbiological and spectroscopicmore » techniques to determine the solubility and phase associations of {sup 99}Tc in FRC sediments, and characterize the underpinning biogeochemical controls.« less

Authors:
; ; ; ; ; ; ;
Publication Date:
Research Org.:
University of Manchester, UK; University of Leeds, UK; Manchester Royal Infirmary, Manchester, UK
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
894940
Report Number(s):
CONF-ERSP2006-71
TRN: US200702%%469
DOE Contract Number:
FG02-04ER63743
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:
54 ENVIRONMENTAL SCIENCES; 59 BASIC BIOLOGICAL SCIENCES; ANAEROBIC CONDITIONS; AQUIFERS; BACTERIA; BIOREMEDIATION; GAMMA CAMERAS; HALF-LIFE; METABOLISM; MICROORGANISMS; POLLUTANTS; PRECIPITATION; PROBES; SEDIMENTS; SOLUBILITY; SULFATES; TECHNETIUM; TECHNETIUM 99; US DOE

Citation Formats

Lloyd, J.R., McBeth, J.M., Lear, G., Morris, K., Burke, I.T., Livens, F.R., Ellis, B., and Lawson, R. Investigation of Technetium Redox Cycling in FRC Background Sediments using EXAFS and Gamma Camera Imaging. United States: N. p., 2006. Web.
Lloyd, J.R., McBeth, J.M., Lear, G., Morris, K., Burke, I.T., Livens, F.R., Ellis, B., & Lawson, R. Investigation of Technetium Redox Cycling in FRC Background Sediments using EXAFS and Gamma Camera Imaging. United States.
Lloyd, J.R., McBeth, J.M., Lear, G., Morris, K., Burke, I.T., Livens, F.R., Ellis, B., and Lawson, R. Wed . "Investigation of Technetium Redox Cycling in FRC Background Sediments using EXAFS and Gamma Camera Imaging". United States. doi:. https://www.osti.gov/servlets/purl/894940.
@article{osti_894940,
title = {Investigation of Technetium Redox Cycling in FRC Background Sediments using EXAFS and Gamma Camera Imaging},
author = {Lloyd, J.R. and McBeth, J.M. and Lear, G. and Morris, K. and Burke, I.T. and Livens, F.R. and Ellis, B. and Lawson, R.},
abstractNote = {Technetium-99 is a priority pollutant at numerous DOE sites, due to its long half-life (2.1 x 105 years), high mobility as Tc(VII) in oxic waters, and bioavailability as a sulfate analogue. {sup 99}Tc is far less mobile under anaerobic conditions, forming insoluble Tc(IV) precipitates. As anaerobic microorganisms can reduce soluble Tc(VII) to insoluble Tc(IV), microbial metabolism may have the potential to treat sediments and waters contaminated with Tc. Baseline studies of fundamental mechanisms of Tc(VII) bioreduction and precipitation (reviewed by Lloyd et al., 2005, in press) have generally used pure cultures of metal-reducing bacteria, in order to develop conceptual models for the biogeochemical cycling of {sup 99}Tc. There is, however, comparatively little known about interactions of metal-reducing bacteria with environmentally relevant trace concentrations of {sup 99}Tc, against a more complex biogeochemical background provided by mixed microbial communities in aquifer sediments. The objective of this project is to probe the site specific biogeochemical conditions that control the mobility of {sup 99}Tc at the US DOE Field Research Center Site (FRC; Oak Ridge, Tennessee). This information is required for the rational design of in situ bioremediation strategies for technetium-contaminated subsurface environments. We are using a combination of geochemical, mineralogical, microbiological and spectroscopic techniques to determine the solubility and phase associations of {sup 99}Tc in FRC sediments, and characterize the underpinning biogeochemical controls.},
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:
Other availability
Please see Document Availability for additional information on obtaining the full-text document. Library patrons may search WorldCat to identify libraries that hold this conference proceeding.

Save / Share:
  • Technetium-99 is a priority pollutant at numerous DOE sites, due to its long half-life (2.1 x 10{sup 5} years), high mobility as Tc(VII) in oxic waters, and bioavailability as a sulfate analog. {sup 99}Tc is far less mobile under anaerobic conditions, forming insoluble Tc(IV) precipitates. As anaerobic microorganisms can reduce soluble Tc(VII) to insoluble Tc(IV), microbial metabolism may have the potential to treat sediments and waters contaminated with Tc. Baseline studies of fundamental mechanisms of Tc(VII) bioreduction and precipitation (reviewed by Lloyd et al, 2002) have generally used pure cultures of metal-reducing bacteria, in order to develop conceptual models formore » the biogeochemical cycling of Tc. There is, however, comparatively little known about interactions of metal-reducing bacteria with environmentally relevant trace concentrations of Tc, against a more complex biogeochemical background provided by mixed microbial communities in the subsurface. The objective of this new NABIR project is to probe the site specific biogeochemical conditions that control the mobility of Tc at the FRC (Oak Ridge, TN). This information is required for the rational design of in situ bioremediation strategies for technetium-contaminated subsurface environments. We will use a combination of geochemical, mineralogical, microbiological and spectroscopic techniques to determine the solubility and phase associations of Tc in FRC sediments, and characterize the underpinning biogeochemical controls. A key strength of this project is that many of the techniques we are using have already been optimized by our research team, who are also studying the biogeochemical controls on Tc mobility in marine and freshwater sediments in the UK in a NERC funded companion study.« less
  • The objective of this research program was to take a highly multidisciplinary approach to define the biogeochemical factors that control technetium (Tc) mobility in FRC sediments. The aim was to use batch and column studies to probe the biogeochemical conditions that control the mobility of Tc at the FRC. Background sediment samples from Area 2 (pH 6.5, low nitrate, low {sup 99}Tc) and Area 3 (pH 3.5, high nitrate, relatively high {sup 99}Tc) of the FRC were selected (http://www.esd.ornl.gov/nabirfrc). For the batch experiments, sediments were mixed with simulated groundwater, modeled on chemical constituents of FRC waters and supplemented with {supmore » 99}Tc(VII), both with and without added electron donor (acetate). The solubility of the Tc was monitored, alongside other biogeochemical markers (nitrate, nitrite, Fe(II), sulfate, acetate, pH, Eh) as the 'microcosms' aged. At key points, the microbial communities were also profiled using both cultivation-dependent and molecular techniques, and results correlated with the geochemical conditions in the sediments. The mineral phases present in the sediments were also characterized, and the solid phase associations of the Tc determined using sequential extraction and synchrotron techniques. In addition to the batch sediment experiments, where discrete microbial communities with the potential to reduce and precipitate {sup 99}Tc will be separated in time, we also developed column experiments where biogeochemical processes were spatially separated. Experiments were conducted both with and without amendments proposed to stimulate radionuclide immobilization (e.g. the addition of acetate as an electron donor for metal reduction), and were also planned with and without competing anions at high concentration (e.g. nitrate, with columns containing Area 3 sediments). When the columns had stabilized, as determined by chemical analysis of the effluents, we used a spike of the short-lived gamma emitter {sup 99m}Tc (50-200 MBq; half life 6 hours) and its mobility was monitored using a {gamma}-camera. Incorporation of low concentrations of the long-lived 99Tc gave a tracer that can be followed by scintillation counting, should the metastable form of the radionuclide decay to below detection limits before the end of the experiment (complete immobilization or loss of the Tc from the column). After the Tc was reduced and immobilized, or passed through the system, the columns were dismantled carefully in an anaerobic cabinet and the pore water geochemistry and mineralogy of the columns profiled. Microbial community analysis was determined, again using molecular and culture-dependent techniques. Experimental results were also modeled using an established coupled speciation and transport code, to develop a predictive tool for the mobility of Tc in FRC sediments. From this multidisciplinary approach, we hoped to obtain detailed information on the microorganisms that control the biogeochemical cycling of key elements at the FRC, and we would also be able to determine the key factors that control the mobility of Tc at environmentally relevant concentrations at this site.« less
  • A variety of methods has been proposed to estimate glomerular filtration rate (GFR) from renal uptake of Tc-99m-DTPA using a gamma camera. To compare alternative methods, the authors have calculated GFR in several different ways from measurements in 33 patients, and compared the results with an independent GFR measurement based on 8-point plasma clearance of Yb-169-DTPA. The best agreement was obtained using an algorithm that has not been described previously. This was a modification of a method used previously in which correction was made for overlap of kidneys by liver and spleen. The correlation coefficient was 0.958 and the residualmore » standard deviation was 12.1 ml/min. This method required a single 20-min blood sample as well as the camera data. The best method not requiring a blood sample was significantly less accurate, with correlation coefficient 0.866 and residual standard deviation 21.1 ml/min. The accuracy of these methods was comparable to that reported for the creatinine clearance, the most commonly used estimate of GFR in current clinical practice.« less
  • The utility of coded aperture ..gamma.. camera imaging of radioisotope distributions in Nuclear Medicine is in its ability to give depth information about a three dimensional source. We have calculated imaging with Fresnel zone plate and multiple pinhole apertures to produce coded shadows and reconstruction of these shadows using correlation, Fresnel diffraction, and Fourier transform deconvolution. Comparisons of the coded apertures and decoding methods are made by evaluating their point response functions both for in-focus and out-of-focus image planes. Background averages and standard deviations were calculated. In some cases, background subtraction was made using combinations of two complementary apertures. Resultsmore » using deconvolution reconstruction for finite numbers of events are also given.« less