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Title: Retention and chemical speciation of uranium in an oxidized wetland sediment from the Savannah River Site

Abstract

Uranium speciation and retention mechanism onto Savannah River Site (SRS) wetland sediments was studied using batch (ad)sorption experiments, sequential extraction desorption tests and U L{sub 3}-edge X-ray absorption near-edge structure (XANES) spectroscopy of contaminated wetland sediments. U was highly retained by the SRS wetland sediments. In contrast to other similar but much lower natural organic matter (NOM) sediments, significant sorption of U onto the SRS sediments was observed at pH <4 and pH >8. Sequential extraction tests indicated that the U(VI) species were primarily associated with the acid soluble fraction (weak acetic acid extractable) and NOM fraction (Na-pyrophosphate extractable). Uranium L3- edge XANES spectra of the U-retained sediments were nearly identical to that of uranyl acetate. The primary oxidation state of U in these sediments was as U(VI), and there was little evidence that the high sorptive capacity of the sediments could be ascribed to abiotic or biotic reduction to the less soluble U(IV) species. The molecular mechanism responsible for the high U retention in the SRS wetland sediments is likely related to the chemical bonding of U to organic carbon.

Authors:
; ; ; ; ; ; ; ; ; ORCiD logo; ; ; ;
Publication Date:
Research Org.:
SRS
Sponsoring Org.:
USDOE
OSTI Identifier:
1108731
Report Number(s):
SRNL-MS-2013-00093
Journal ID: ISSN 0265-931X
DOE Contract Number:  
DE-AC09-08SR22470
Resource Type:
Journal Article
Journal Name:
Journal of Environmental Radioactivity
Additional Journal Information:
Journal Volume: 131; Journal ID: ISSN 0265-931X
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES; Wetland sediments, uranium, chemical speciation, retention

Citation Formats

Li, Dien, Seaman, John C., Chang, Hyun-Shik, Jaffe, Peter R., Koster van Groos, Paul, Jiang, De-Tong, Chen, Ning, Lin, Jinru, Arthur, Zachary, Pan, Yuanming, Scheckel, Kirk G., Newville, Matthew, Lanzirotti, Antonio, and Kaplan, Daniel I. Retention and chemical speciation of uranium in an oxidized wetland sediment from the Savannah River Site. United States: N. p., 2014. Web. doi:10.1016/j.jenvrad.2013.10.017.
Li, Dien, Seaman, John C., Chang, Hyun-Shik, Jaffe, Peter R., Koster van Groos, Paul, Jiang, De-Tong, Chen, Ning, Lin, Jinru, Arthur, Zachary, Pan, Yuanming, Scheckel, Kirk G., Newville, Matthew, Lanzirotti, Antonio, & Kaplan, Daniel I. Retention and chemical speciation of uranium in an oxidized wetland sediment from the Savannah River Site. United States. doi:10.1016/j.jenvrad.2013.10.017.
Li, Dien, Seaman, John C., Chang, Hyun-Shik, Jaffe, Peter R., Koster van Groos, Paul, Jiang, De-Tong, Chen, Ning, Lin, Jinru, Arthur, Zachary, Pan, Yuanming, Scheckel, Kirk G., Newville, Matthew, Lanzirotti, Antonio, and Kaplan, Daniel I. Thu . "Retention and chemical speciation of uranium in an oxidized wetland sediment from the Savannah River Site". United States. doi:10.1016/j.jenvrad.2013.10.017. https://www.osti.gov/servlets/purl/1108731.
@article{osti_1108731,
title = {Retention and chemical speciation of uranium in an oxidized wetland sediment from the Savannah River Site},
author = {Li, Dien and Seaman, John C. and Chang, Hyun-Shik and Jaffe, Peter R. and Koster van Groos, Paul and Jiang, De-Tong and Chen, Ning and Lin, Jinru and Arthur, Zachary and Pan, Yuanming and Scheckel, Kirk G. and Newville, Matthew and Lanzirotti, Antonio and Kaplan, Daniel I.},
abstractNote = {Uranium speciation and retention mechanism onto Savannah River Site (SRS) wetland sediments was studied using batch (ad)sorption experiments, sequential extraction desorption tests and U L{sub 3}-edge X-ray absorption near-edge structure (XANES) spectroscopy of contaminated wetland sediments. U was highly retained by the SRS wetland sediments. In contrast to other similar but much lower natural organic matter (NOM) sediments, significant sorption of U onto the SRS sediments was observed at pH <4 and pH >8. Sequential extraction tests indicated that the U(VI) species were primarily associated with the acid soluble fraction (weak acetic acid extractable) and NOM fraction (Na-pyrophosphate extractable). Uranium L3- edge XANES spectra of the U-retained sediments were nearly identical to that of uranyl acetate. The primary oxidation state of U in these sediments was as U(VI), and there was little evidence that the high sorptive capacity of the sediments could be ascribed to abiotic or biotic reduction to the less soluble U(IV) species. The molecular mechanism responsible for the high U retention in the SRS wetland sediments is likely related to the chemical bonding of U to organic carbon.},
doi = {10.1016/j.jenvrad.2013.10.017},
journal = {Journal of Environmental Radioactivity},
issn = {0265-931X},
number = ,
volume = 131,
place = {United States},
year = {2014},
month = {5}
}