Spectroscopic evidence of uranium immobilization in acidic wetlands by natural organic matter and plant roots

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

doi:10.1021/ES505369G

Spectroscopic evidence of uranium immobilization in acidic wetlands by natural organic matter and plant roots

Journal Article · Tue Mar 03 00:00:00 EST 2015 · Environmental Science and Technology

DOI:https://doi.org/10.1021/ES505369G· OSTI ID:1174137

Li, Dien ^[1]; Kaplan, Daniel I. ^[1]; Chang, Hyun-Shik ^[2]; Seaman, John C. ^[2]; Jaffé, Peter R. ^[3]; Koster van Groos, Paul ^[3]; Scheckel, Kirk G. ^[4]; Segre, Carlo U. ^[5]; Chen, Ning ^[6]; Jiang, De-Tong ^[7]; Newville, Matthew ^[8]; Lanzirotti, Antonio ^[8]

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)

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.

View Accepted Manuscript (DOE)

Research Organization:: Savannah River Site (SRS), Aiken, SC (United States)

Sponsoring Organization:: Office of Environmental Management (EM); USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23)

Grant/Contract Number:: AC02-06CH11357; AC09-08SR22470; AC09-96SR18500; FC09-07SR22506; FG02-94ER14466; SC0006847

OSTI ID:: 1174137

Alternate ID(s):: OSTI ID: 1172416

Report Number(s):: SRNS-STI--2015-00177

Journal Information:: Environmental Science and Technology, Journal Name: Environmental Science and Technology Journal Issue: 5 Vol. 49; ISSN 0013-936X

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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