Spectroscopic evidence of uranium immobilization in acidic wetlands by natural organic matter and plant roots
Abstract
Biogeochemistry of uranium in wetlands plays important roles in U immobilization in storage ponds of U mining and processing facilities but has not been well understood. The objective of this work was to study molecular mechanisms responsible for high U retention by Savannah River Site (SRS) wetland sediments under varying redox and acidic (pH = 2.6–5.8) conditions using U L₃-edge X-ray absorption spectroscopy. Uranium in the SRS wetland sediments existed primarily as U(VI) bonded as a bidentate to carboxylic sites (U–C bond distance at ~2.88 Å), rather than phenolic or other sites of natural organic matter (NOM). In microcosms simulating the SRS wetland processes, U immobilization on roots was two orders of magnitude higher than on the adjacent brown or more distant white sands in which U was U(VI). Uranium on the roots were both U(IV) and U(VI), which were bonded as a bidentate to carbon, but the U(VI) may also form a U phosphate mineral. After 140 days of air exposure, all U(IV) was re-oxidized to U(VI) but remained as a bidentate bonding to carbon. This study demonstrated NOM and plant roots can highly immobilize U(VI) in the SRS acidic sediments, which has significant implication for the long-term stewardshipmore »
- Authors:
-
- Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL)
- Savannah River Site (SRS), Aiken, SC (United States). Savannah River Ecology Lab. (SREL)
- Princeton Univ., NJ (United States). Dept. of Civil and Environmental Engineering
- US Environmental Protection Agency (EPA), Cincinnati, OH (United States). National Risk Management Research Lab.
- Illinois Inst. of Technology, Chicago, IL (United States). Physics Dept. and CSRRI
- Canadian Light Sources, Inc., Saskatoon, SK (Canada)
- Univ. of Guelph, ON (Canada). Dept. of Physics
- Univ. of Chicago, IL (United States). Center for Advanced Radiation Sources (CARS)
- Publication Date:
- Research Org.:
- Savannah River Site (SRS), Aiken, SC (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Biological and Environmental Research (BER); Office of Environmental Management (EM)
- OSTI Identifier:
- 1174137
- Report Number(s):
- SRNS-STI-2015-00177
Journal ID: ISSN 0013-936X
- Grant/Contract Number:
- AC09-96SR18500; FC09-07SR22506; AC09-08SR22470; SC0006847; AC02-06CH11357; FG02-94ER14466
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Environmental Science and Technology
- Additional Journal Information:
- Journal Volume: 49; Journal Issue: 5; Journal ID: ISSN 0013-936X
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 58 GEOSCIENCES; 54 ENVIRONMENTAL SCIENCES; ray-absorption-spectroscopy; savanna river site; in-situ; contaminated sediments; hydroxyapatite addition; chemical speciation; reducing conditions; u(vi) bioreduction; humic acids; reduction
Citation Formats
Li, Dien, Kaplan, Daniel I., Chang, Hyun-Shik, Seaman, John C., Jaffé, Peter R., Koster van Groos, Paul, Scheckel, Kirk G., Segre, Carlo U., Chen, Ning, Jiang, De-Tong, Newville, Matthew, and Lanzirotti, Antonio. Spectroscopic evidence of uranium immobilization in acidic wetlands by natural organic matter and plant roots. United States: N. p., 2015.
Web. doi:10.1021/ES505369G.
Li, Dien, Kaplan, Daniel I., Chang, Hyun-Shik, Seaman, John C., Jaffé, Peter R., Koster van Groos, Paul, Scheckel, Kirk G., Segre, Carlo U., Chen, Ning, Jiang, De-Tong, Newville, Matthew, & Lanzirotti, Antonio. Spectroscopic evidence of uranium immobilization in acidic wetlands by natural organic matter and plant roots. United States. https://doi.org/10.1021/ES505369G
Li, Dien, Kaplan, Daniel I., Chang, Hyun-Shik, Seaman, John C., Jaffé, Peter R., Koster van Groos, Paul, Scheckel, Kirk G., Segre, Carlo U., Chen, Ning, Jiang, De-Tong, Newville, Matthew, and Lanzirotti, Antonio. Tue .
"Spectroscopic evidence of uranium immobilization in acidic wetlands by natural organic matter and plant roots". United States. https://doi.org/10.1021/ES505369G. https://www.osti.gov/servlets/purl/1174137.
@article{osti_1174137,
title = {Spectroscopic evidence of uranium immobilization in acidic wetlands by natural organic matter and plant roots},
author = {Li, Dien and Kaplan, Daniel I. and Chang, Hyun-Shik and Seaman, John C. and Jaffé, Peter R. and Koster van Groos, Paul and Scheckel, Kirk G. and Segre, Carlo U. and Chen, Ning and Jiang, De-Tong and Newville, Matthew and Lanzirotti, Antonio},
abstractNote = {Biogeochemistry of uranium in wetlands plays important roles in U immobilization in storage ponds of U mining and processing facilities but has not been well understood. The objective of this work was to study molecular mechanisms responsible for high U retention by Savannah River Site (SRS) wetland sediments under varying redox and acidic (pH = 2.6–5.8) conditions using U L₃-edge X-ray absorption spectroscopy. Uranium in the SRS wetland sediments existed primarily as U(VI) bonded as a bidentate to carboxylic sites (U–C bond distance at ~2.88 Å), rather than phenolic or other sites of natural organic matter (NOM). In microcosms simulating the SRS wetland processes, U immobilization on roots was two orders of magnitude higher than on the adjacent brown or more distant white sands in which U was U(VI). Uranium on the roots were both U(IV) and U(VI), which were bonded as a bidentate to carbon, but the U(VI) may also form a U phosphate mineral. After 140 days of air exposure, all U(IV) was re-oxidized to U(VI) but remained as a bidentate bonding to carbon. This study demonstrated NOM and plant roots can highly immobilize U(VI) in the SRS acidic sediments, which has significant implication for the long-term stewardship of U-contaminated wetlands.},
doi = {10.1021/ES505369G},
journal = {Environmental Science and Technology},
number = 5,
volume = 49,
place = {United States},
year = {2015},
month = {3}
}
Web of Science
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