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Title: Pilot-Scale In Situ Bioremediation of Uranium in a Highly Contaminated Aquifer. 2. Reduction of U(VI and Geochemical Control of U(VI) Bioavailability

Abstract

In situ microbial reduction of soluble U(VI) to sparingly soluble U(IV) was evaluated at the site of the former S-3 Ponds in Area 3 of the U.S. Department of Energy Natural and Accelerated Bioremediation Research Field Research Center, Oak Ridge, TN. After establishing conditions favorable for bioremediation (Wu, et al. Environ. Sci. Technol. 2006, 40, 3988-3995), intermittent additions of ethanol were initiated within the conditioned inner loop of a nested well recirculation system. These additions initially stimulated denitrification of matrix-entrapped nitrate, but after 2 months, aqueous U levels fell from 5 to {approx}1 {micro}M and sulfate reduction ensued. Continued additions sustained U(VI) reduction over 13 months. X-ray near-edge absorption spectroscopy (XANES) confirmed U(VI) reduction to U(IV) within the inner loop wells, with up to 51%, 35%, and 28% solid-phase U(IV) in sediment samples from the injection well, a monitoring well, and the extraction well, respectively. Microbial analyses confirmed the presence of denitrifying, sulfate-reducing, and iron-reducing bacteria in groundwater and sediments. System pH was generally maintained at less than 6.2 with low bicarbonate level (0.75-1.5 mM) and residual sulfate to suppress methanogenesis and minimize uranium mobilization. The bioavailability of sorbed U(VI) was manipulated by addition of low-level carbonate (<5 mM) followedmore » by ethanol (1-1.5 mM). Addition of low levels of carbonate increased the concentration of aqueous U, indicating an increased rate of U desorption due to formation of uranyl carbonate complexes. Upon ethanol addition, aqueous U(VI) levels fell, indicating that the rate of microbial reduction exceeded the rate of desorption. Sulfate levels simultaneously decreased, with a corre sponding increase in sulfide. When ethanol addition ended but carbonate addition continued, soluble U levels increased, indicating faster desorption than reduction. When bicarbonate addition stopped, aqueous U levels decreased, indicating adsorption to sediments. Changes in the sequence of carbonate and ethanol addition confirmed that carbonate-controlled desorption increased bioavailability of U(VI) for reduction.« less

Authors:
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  1. ORNL
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
989669
DOE Contract Number:  
DE-AC05-00OR22725
Resource Type:
Journal Article
Journal Name:
Environmental Science & Technology
Additional Journal Information:
Journal Volume: 40; Journal Issue: 12; Journal ID: ISSN 0013-936X
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES; ABSORPTION SPECTROSCOPY; ACID CARBONATES; ADSORPTION; BACTERIA; BIOREMEDIATION; CARBONATES; DENITRIFICATION; DESORPTION; ETHANOL; INJECTION WELLS; MONITORING; PONDS; SEDIMENTS; SULFATES; URANIUM; URANYL CARBONATES

Citation Formats

Wu, Weimin, Carley, Jack M, Gentry, Terry J, Ginder-Vogel, Matthew, Fienen, Michael, Mehlhorn, Tonia L, Yan, Hui, Carroll, Sue L, Pace, Molly, Nyman, Jennifer L, Luo, Jian, Fields, Matthew Wayne, Hickey, Robert, Gu, Baohua, Watson, David B, Cirpka, Olaf, Zhou, Jizhong, Fendorf, Scott, Kitanidis, Peter K, Jardine, Philip M, and Criddle, Craig. Pilot-Scale In Situ Bioremediation of Uranium in a Highly Contaminated Aquifer. 2. Reduction of U(VI and Geochemical Control of U(VI) Bioavailability. United States: N. p., 2006. Web. doi:10.1021/es051960u.
Wu, Weimin, Carley, Jack M, Gentry, Terry J, Ginder-Vogel, Matthew, Fienen, Michael, Mehlhorn, Tonia L, Yan, Hui, Carroll, Sue L, Pace, Molly, Nyman, Jennifer L, Luo, Jian, Fields, Matthew Wayne, Hickey, Robert, Gu, Baohua, Watson, David B, Cirpka, Olaf, Zhou, Jizhong, Fendorf, Scott, Kitanidis, Peter K, Jardine, Philip M, & Criddle, Craig. Pilot-Scale In Situ Bioremediation of Uranium in a Highly Contaminated Aquifer. 2. Reduction of U(VI and Geochemical Control of U(VI) Bioavailability. United States. https://doi.org/10.1021/es051960u
Wu, Weimin, Carley, Jack M, Gentry, Terry J, Ginder-Vogel, Matthew, Fienen, Michael, Mehlhorn, Tonia L, Yan, Hui, Carroll, Sue L, Pace, Molly, Nyman, Jennifer L, Luo, Jian, Fields, Matthew Wayne, Hickey, Robert, Gu, Baohua, Watson, David B, Cirpka, Olaf, Zhou, Jizhong, Fendorf, Scott, Kitanidis, Peter K, Jardine, Philip M, and Criddle, Craig. 2006. "Pilot-Scale In Situ Bioremediation of Uranium in a Highly Contaminated Aquifer. 2. Reduction of U(VI and Geochemical Control of U(VI) Bioavailability". United States. https://doi.org/10.1021/es051960u.
@article{osti_989669,
title = {Pilot-Scale In Situ Bioremediation of Uranium in a Highly Contaminated Aquifer. 2. Reduction of U(VI and Geochemical Control of U(VI) Bioavailability},
author = {Wu, Weimin and Carley, Jack M and Gentry, Terry J and Ginder-Vogel, Matthew and Fienen, Michael and Mehlhorn, Tonia L and Yan, Hui and Carroll, Sue L and Pace, Molly and Nyman, Jennifer L and Luo, Jian and Fields, Matthew Wayne and Hickey, Robert and Gu, Baohua and Watson, David B and Cirpka, Olaf and Zhou, Jizhong and Fendorf, Scott and Kitanidis, Peter K and Jardine, Philip M and Criddle, Craig},
abstractNote = {In situ microbial reduction of soluble U(VI) to sparingly soluble U(IV) was evaluated at the site of the former S-3 Ponds in Area 3 of the U.S. Department of Energy Natural and Accelerated Bioremediation Research Field Research Center, Oak Ridge, TN. After establishing conditions favorable for bioremediation (Wu, et al. Environ. Sci. Technol. 2006, 40, 3988-3995), intermittent additions of ethanol were initiated within the conditioned inner loop of a nested well recirculation system. These additions initially stimulated denitrification of matrix-entrapped nitrate, but after 2 months, aqueous U levels fell from 5 to {approx}1 {micro}M and sulfate reduction ensued. Continued additions sustained U(VI) reduction over 13 months. X-ray near-edge absorption spectroscopy (XANES) confirmed U(VI) reduction to U(IV) within the inner loop wells, with up to 51%, 35%, and 28% solid-phase U(IV) in sediment samples from the injection well, a monitoring well, and the extraction well, respectively. Microbial analyses confirmed the presence of denitrifying, sulfate-reducing, and iron-reducing bacteria in groundwater and sediments. System pH was generally maintained at less than 6.2 with low bicarbonate level (0.75-1.5 mM) and residual sulfate to suppress methanogenesis and minimize uranium mobilization. The bioavailability of sorbed U(VI) was manipulated by addition of low-level carbonate (<5 mM) followed by ethanol (1-1.5 mM). Addition of low levels of carbonate increased the concentration of aqueous U, indicating an increased rate of U desorption due to formation of uranyl carbonate complexes. Upon ethanol addition, aqueous U(VI) levels fell, indicating that the rate of microbial reduction exceeded the rate of desorption. Sulfate levels simultaneously decreased, with a corre sponding increase in sulfide. When ethanol addition ended but carbonate addition continued, soluble U levels increased, indicating faster desorption than reduction. When bicarbonate addition stopped, aqueous U levels decreased, indicating adsorption to sediments. Changes in the sequence of carbonate and ethanol addition confirmed that carbonate-controlled desorption increased bioavailability of U(VI) for reduction.},
doi = {10.1021/es051960u},
url = {https://www.osti.gov/biblio/989669}, journal = {Environmental Science & Technology},
issn = {0013-936X},
number = 12,
volume = 40,
place = {United States},
year = {Sat Jul 01 00:00:00 EDT 2006},
month = {Sat Jul 01 00:00:00 EDT 2006}
}