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Title: Effects of aqueous uranyl speciation on the kinetics of microbial uranium reduction

Abstract

The ability to predict the success of the microbial reduction of soluble U(VI) to highly insoluble U(IV) as an in situ bioremediation strategy is complicated by the wide range of geochemical conditions at contaminated sites and the strong influence of aqueous uranyl speciation on the bioavailability and toxicity of U(VI) to metal-reducing bacteria. In order to determine the effects of aqueous uranyl speciation on uranium bioreduction kinetics, incubations and viability assays with Shewanella putrefaciens strain 200 were conducted over a range of pH and dissolved inorganic carbon (DIC), Ca2+, and Mg2+ concentrations. A speciation-dependent kinetic model was developed to reproduce the observed time series of total dissolved uranium concentration over the range of geochemical conditions tested. The kinetic model yielded the highest rate constant for the reduction of uranyl non-carbonate species (i.e., the ‘free’ hydrated uranyl ion, uranyl hydroxides, and other minor uranyl complexes), indicating that they represent the most readily reducible fraction of U(VI) despite being the least abundant uranyl species in solution. In the presence of DIC, Ca2+, and Mg2+ is suppressed during the formation of more bioavailable uranyl non-carbonate species and resulted in slower bioreduction rates. At high concentrations of bioavailable U(VI), however, uranium toxicity to S.more » putrefaciens inhibited bioreduction, and viability assays confirmed that the concentration of non-carbonate uranyl species best predicts the degree of toxicity. The effect of uranium toxicity was accounted for by incorporating the free ion activity model of metal toxicity into the bioreduction rate law. These results demonstrate that, in the absence of competing terminal electron acceptors, uranium bioreduction kinetics can be predicted over a wide range of geochemical conditions based on the bioavailability and toxicity imparted on U(VI) by solution composition. Finally, these findings also imply that the concentration of uranyl non-carbonate species, despite being extremely low, is a determining factor controlling uranium bioreduction at contaminated sites.« less

Authors:
 [1];  [2];  [3];  [1]
+ Show Author Affiliations
  1. Georgia Inst. of Technology, Atlanta, GA (United States). School of Earth and Atmospheric Sciences
  2. Georgia Inst. of Technology, Atlanta, GA (United States). School of Biology
  3. Univ. of Waterloo, ON (Canada). Dept. of Earth and Environmental Sciences and Water Inst.
Publication Date:
Research Org.:
Georgia Institute of Technology, Atlanta, GA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER)
OSTI Identifier:
1332077
Alternate Identifier(s):
OSTI ID: 1246405
Grant/Contract Number:  
SC0005520
Resource Type:
Accepted Manuscript
Journal Name:
Geochimica et Cosmochimica Acta
Additional Journal Information:
Journal Volume: 157; Journal Issue: C; Journal ID: ISSN 0016-7037
Publisher:
The Geochemical Society; The Meteoritical Society
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES; 58 GEOSCIENCES; 12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE WASTES FROM NUCLEAR FACILITIES; Uranium bioreduction; uranium bioavailability; uranium speciation; uranium toxicity; uranium bioremediation

Citation Formats

Belli, Keaton M., DiChristina, Thomas J., Van Cappellen, Philippe, and Taillefert, Martial. Effects of aqueous uranyl speciation on the kinetics of microbial uranium reduction. United States: N. p., 2015. Web. doi:10.1016/j.gca.2015.02.006.
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Belli, Keaton M., DiChristina, Thomas J., Van Cappellen, Philippe, & Taillefert, Martial. Effects of aqueous uranyl speciation on the kinetics of microbial uranium reduction. United States. https://doi.org/10.1016/j.gca.2015.02.006
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Belli, Keaton M., DiChristina, Thomas J., Van Cappellen, Philippe, and Taillefert, Martial. Mon . "Effects of aqueous uranyl speciation on the kinetics of microbial uranium reduction". United States. https://doi.org/10.1016/j.gca.2015.02.006. https://www.osti.gov/servlets/purl/1332077.
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@article{osti_1332077,
title = {Effects of aqueous uranyl speciation on the kinetics of microbial uranium reduction},
author = {Belli, Keaton M. and DiChristina, Thomas J. and Van Cappellen, Philippe and Taillefert, Martial},
abstractNote = {The ability to predict the success of the microbial reduction of soluble U(VI) to highly insoluble U(IV) as an in situ bioremediation strategy is complicated by the wide range of geochemical conditions at contaminated sites and the strong influence of aqueous uranyl speciation on the bioavailability and toxicity of U(VI) to metal-reducing bacteria. In order to determine the effects of aqueous uranyl speciation on uranium bioreduction kinetics, incubations and viability assays with Shewanella putrefaciens strain 200 were conducted over a range of pH and dissolved inorganic carbon (DIC), Ca2+, and Mg2+ concentrations. A speciation-dependent kinetic model was developed to reproduce the observed time series of total dissolved uranium concentration over the range of geochemical conditions tested. The kinetic model yielded the highest rate constant for the reduction of uranyl non-carbonate species (i.e., the ‘free’ hydrated uranyl ion, uranyl hydroxides, and other minor uranyl complexes), indicating that they represent the most readily reducible fraction of U(VI) despite being the least abundant uranyl species in solution. In the presence of DIC, Ca2+, and Mg2+ is suppressed during the formation of more bioavailable uranyl non-carbonate species and resulted in slower bioreduction rates. At high concentrations of bioavailable U(VI), however, uranium toxicity to S. putrefaciens inhibited bioreduction, and viability assays confirmed that the concentration of non-carbonate uranyl species best predicts the degree of toxicity. The effect of uranium toxicity was accounted for by incorporating the free ion activity model of metal toxicity into the bioreduction rate law. These results demonstrate that, in the absence of competing terminal electron acceptors, uranium bioreduction kinetics can be predicted over a wide range of geochemical conditions based on the bioavailability and toxicity imparted on U(VI) by solution composition. Finally, these findings also imply that the concentration of uranyl non-carbonate species, despite being extremely low, is a determining factor controlling uranium bioreduction at contaminated sites.},
doi = {10.1016/j.gca.2015.02.006},
journal = {Geochimica et Cosmochimica Acta},
number = C,
volume = 157,
place = {United States},
year = {Mon Feb 16 00:00:00 EST 2015},
month = {Mon Feb 16 00:00:00 EST 2015}
}
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