skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: 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 » of U-contaminated wetlands.« less

Authors:
 [1];  [1];  [2];  [2];  [3];  [3];  [4];  [5];  [6];  [7];  [8];  [8]
  1. Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL)
  2. Savannah River Site (SRS), Aiken, SC (United States). Savannah River Ecology Lab. (SREL)
  3. Princeton Univ., NJ (United States). Dept. of Civil and Environmental Engineering
  4. US Environmental Protection Agency (EPA), Cincinnati, OH (United States). National Risk Management Research Lab.
  5. Illinois Inst. of Technology, Chicago, IL (United States). Physics Dept. and CSRRI
  6. Canadian Light Sources, Inc., Saskatoon, SK (Canada)
  7. Univ. of Guelph, ON (Canada). Dept. of Physics
  8. 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. 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, & 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}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 10 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

In situ Chemical Speciation of Uranium in Soils and Sediments by Micro X-ray Absorption Spectroscopy
journal, May 1994

  • Bertsch, Paul M.; Hunter, Douglas B.; Sutton, Stephen R.
  • Environmental Science & Technology, Vol. 28, Issue 5
  • DOI: 10.1021/es00054a034

Retention and chemical speciation of uranium in an oxidized wetland sediment from the Savannah River Site
journal, May 2014


Quantification of thorium and uranium sorption to contaminated sediments
journal, June 2004

  • Kaplan, D. I.; Serkiz, S. M.
  • Journal of Radioanalytical and Nuclear Chemistry, Vol. 248, Issue 3, p. 529-535
  • DOI: 10.1023/A:1010606325979

Partitioning and Availability of Uranium and Nickel in Contaminated Riparian Sediments
journal, January 2003

  • Sowder, Andrew G.; Bertsch, Paul M.; Morris, Pamela J.
  • Journal of Environment Quality, Vol. 32, Issue 3
  • DOI: 10.2134/jeq2003.8850

Immobilization of Nickel and Other Metals in Contaminated Sediments by Hydroxyapatite Addition
journal, January 2001

  • Seaman, John C.; Arey, J. Samuel; Bertsch, Paul M.
  • Journal of Environment Quality, Vol. 30, Issue 2
  • DOI: 10.2134/jeq2001.302460x

Method to Attenuate U(VI) Mobility in Acidic Waste Plumes Using Humic Acids
journal, March 2011

  • Wan, Jiamin; Dong, Wenming; Tokunaga, Tetsu K.
  • Environmental Science & Technology, Vol. 45, Issue 6
  • DOI: 10.1021/es103864t

Phytoextraction of uranium and thorium by native trees in a contaminated wetland
journal, May 2005


Elevated uptake of Th and U by netted chain fern (Woodwardia areolata)
journal, April 2008

  • Knox, A. S.; Kaplan, D. I.; Hinton, T. G.
  • Journal of Radioanalytical and Nuclear Chemistry, Vol. 277, Issue 1
  • DOI: 10.1007/s10967-008-0726-3

In situ uranium stabilization by microbial metabolites
journal, June 2008

  • Turick, Charles E.; Knox, Anna S.; Leverette, Chad L.
  • Journal of Environmental Radioactivity, Vol. 99, Issue 6
  • DOI: 10.1016/j.jenvrad.2007.11.020

The product of microbial uranium reduction includes multiple species with U(IV)–phosphate coordination
journal, April 2014

  • Alessi, Daniel S.; Lezama-Pacheco, Juan S.; Stubbs, Joanne E.
  • Geochimica et Cosmochimica Acta, Vol. 131
  • DOI: 10.1016/j.gca.2014.01.005

Quantitative Separation of Monomeric U(IV) from UO 2 in Products of U(VI) Reduction
journal, May 2012

  • Alessi, Daniel S.; Uster, Benjamin; Veeramani, Harish
  • Environmental Science & Technology, Vol. 46, Issue 11
  • DOI: 10.1021/es204123z

Uranium redox transition pathways in acetate-amended sediments
journal, March 2013

  • Bargar, J. R.; Williams, K. H.; Campbell, K. M.
  • Proceedings of the National Academy of Sciences, Vol. 110, Issue 12
  • DOI: 10.1073/pnas.1219198110

Speciation of Uranium in Sediments before and after In situ Biostimulation
journal, March 2008

  • Kelly, Shelly D.; Kemner, Kenneth M.; Carley, Jack
  • Environmental Science & Technology, Vol. 42, Issue 5
  • DOI: 10.1021/es071764i

Uranium Redox Cycling in Sediment and Biomineral Systems
journal, June 2011


Abiotic reduction of uranium by Fe(II) in soil
journal, August 2012


XAFS Investigation of the Interactions of U VI with Secondary Mineralization Products from the Bioreduction of Fe III Oxides
journal, March 2010

  • O’Loughlin, Edward J.; Kelly, Shelly D.; Kemner, Kenneth M.
  • Environmental Science & Technology, Vol. 44, Issue 5
  • DOI: 10.1021/es9027953

Bioreduction of Hydrogen Uranyl Phosphate: Mechanisms and U(IV) Products
journal, May 2013

  • Rui, Xue; Kwon, Man Jae; O’Loughlin, Edward J.
  • Environmental Science & Technology, Vol. 47, Issue 11
  • DOI: 10.1021/es305258p

The role of anaerobic respiration in the immobilization of uranium through biomineralization of phosphate minerals
journal, April 2013

  • Salome, Kathleen R.; Green, Stefan J.; Beazley, Melanie J.
  • Geochimica et Cosmochimica Acta, Vol. 106
  • DOI: 10.1016/j.gca.2012.12.037

Uranium speciation and stability after reductive immobilization in aquifer sediments
journal, November 2011

  • Sharp, Jonathan O.; Lezama-Pacheco, Juan S.; Schofield, Eleanor J.
  • Geochimica et Cosmochimica Acta, Vol. 75, Issue 21
  • DOI: 10.1016/j.gca.2011.08.022

Structural Similarities between Biogenic Uraninites Produced by Phylogenetically and Metabolically Diverse Bacteria
journal, November 2009

  • Sharp, Jonathan O.; Schofield, Eleanor J.; Veeramani, Harish
  • Environmental Science & Technology, Vol. 43, Issue 21
  • DOI: 10.1021/es901281e

Biogeochemical Controls on the Product of Microbial U(VI) Reduction
journal, October 2013

  • Stylo, Malgorzata; Alessi, Daniel S.; Shao, Paul PaoYun
  • Environmental Science & Technology, Vol. 47, Issue 21
  • DOI: 10.1021/es402631w

Nanometre-size products of uranium bioreduction
journal, September 2002

  • Suzuki, Yohey; Kelly, Shelly D.; Kemner, Kenneth M.
  • Nature, Vol. 419, Issue 6903
  • DOI: 10.1038/419134a

U(VI) Bioreduction with Emulsified Vegetable Oil as the Electron Donor – Model Application to a Field Test
journal, March 2013

  • Tang, Guoping; Watson, David B.; Wu, Wei-Min
  • Environmental Science & Technology, Vol. 47, Issue 7
  • DOI: 10.1021/es304643h

Real-Time X-ray Absorption Spectroscopy of Uranium, Iron, and Manganese in Contaminated Sediments During Bioreduction
journal, April 2008

  • Tokunaga, Tetsu K.; Wan, Jiamin; Kim, Yongman
  • Environmental Science & Technology, Vol. 42, Issue 8
  • DOI: 10.1021/es702364x

Abiotic Reductive Immobilization of U(VI) by Biogenic Mackinawite
journal, February 2013

  • Veeramani, Harish; Scheinost, Andreas C.; Monsegue, Niven
  • Environmental Science & Technology, Vol. 47, Issue 5
  • DOI: 10.1021/es304025x

In Situ Bioreduction of Uranium (VI) to Submicromolar Levels and Reoxidation by Dissolved Oxygen
journal, August 2007

  • Wu, Wei-Min; Carley, Jack; Luo, Jian
  • Environmental Science & Technology, Vol. 41, Issue 16
  • DOI: 10.1021/es062657b

The effect of U(VI) bioreduction kinetics on subsequent reoxidation of biogenic U(IV)
journal, October 2007

  • Senko, John M.; Kelly, Shelly D.; Dohnalkova, Alice C.
  • Geochimica et Cosmochimica Acta, Vol. 71, Issue 19
  • DOI: 10.1016/j.gca.2007.07.021

Reoxidation of Bioreduced Uranium under Reducing Conditions
journal, August 2005

  • Wan, Jiamin; Tokunaga, Tetsu K.; Brodie, Eoin
  • Environmental Science & Technology, Vol. 39, Issue 16
  • DOI: 10.1021/es048236g

The role of biogeochemical processes in minimising uranium dispersion from a mine site
journal, February 1997


Geochemistry of natural wetlands in former uranium milling sites (eastern Germany) and implications for uranium retention
journal, February 2009


Uranium Immobilization in an Iron-Rich Rhizosphere of a Native Wetland Plant from the Savannah River Site under Reducing Conditions
journal, July 2014

  • Chang, Hyun-shik; Buettner, Shea W.; Seaman, John. C.
  • Environmental Science & Technology, Vol. 48, Issue 16
  • DOI: 10.1021/es5015136

X-ray absorption fine structure determination of pH-dependent U-bacterial cell wall interactions
journal, November 2002


The New MRCAT (Sector 10) Bending Magnet Beamline at the Advanced Photon Source
conference, January 2010

  • Kropf, A. J.; Katsoudas, J.; Chattopadhyay, S.
  • SRI 2009, 10TH INTERNATIONAL CONFERENCE ON RADIATION INSTRUMENTATION, AIP Conference Proceedings
  • DOI: 10.1063/1.3463194

ATHENA , ARTEMIS , HEPHAESTUS : data analysis for X-ray absorption spectroscopy using IFEFFIT
journal, June 2005


Uranium Transformations in Static Microcosms
journal, January 2010

  • Kelly, Shelly D.; Wu, Wei-Min; Yang, Fan
  • Environmental Science & Technology, Vol. 44, Issue 1
  • DOI: 10.1021/es902191s

Redetermination and absolute configuration of sodium uranyl(VI) triacetate
journal, October 1985

  • Templeton, D. H.; Zalkin, A.; Ruben, H.
  • Acta Crystallographica Section C Crystal Structure Communications, Vol. 41, Issue 10
  • DOI: 10.1107/S0108270185008095

Hydrogen uranyl phosphate tetrahydrate, a hydrogen ion solid electrolyte
journal, December 1978

  • Morosin, B.
  • Acta Crystallographica Section B Structural Crystallography and Crystal Chemistry, Vol. 34, Issue 12
  • DOI: 10.1107/S0567740878011991

In situ study of the goethite-hematite phase transformation by real time synchrotron powder diffraction
journal, June 1999

  • Gualtieri, Alessandro F.; Venturelli, Paolo
  • American Mineralogist, Vol. 84, Issue 5-6
  • DOI: 10.2138/am-1999-5-624

Molecular-Scale Characterization of Uranium Sorption by Bone Apatite Materials for a Permeable Reactive Barrier Demonstration
journal, October 2003

  • Fuller, C. C.; Bargar, J. R.; Davis, J. A.
  • Environmental Science & Technology, Vol. 37, Issue 20
  • DOI: 10.1021/es0343959

Mechanisms of Uranium Interactions with Hydroxyapatite:  Implications for Groundwater Remediation
journal, January 2002

  • Fuller, C. C.; Bargar, J. R.; Davis, J. A.
  • Environmental Science & Technology, Vol. 36, Issue 2
  • DOI: 10.1021/es0108483

Uranyl adsorption and surface speciation at the imogolite–water interface: Self-consistent spectroscopic and surface complexation models
journal, May 2006


Influence of humic acids on the actinide migration in the environment: suitable humic acid model substances and their application in studies with uranium—a review
journal, April 2011

  • Sachs, Susanne; Bernhard, Gert
  • Journal of Radioanalytical and Nuclear Chemistry, Vol. 290, Issue 1
  • DOI: 10.1007/s10967-011-1084-0

Stable U(IV) Complexes Form at High-Affinity Mineral Surface Sites
journal, January 2014

  • Latta, Drew E.; Mishra, Bhoopesh; Cook, Russell E.
  • Environmental Science & Technology, Vol. 48, Issue 3
  • DOI: 10.1021/es4047389

Extracellular reduction of uranium via Geobacter conductive pili as a protective cellular mechanism
journal, September 2011

  • Cologgi, D. L.; Lampa-Pastirk, S.; Speers, A. M.
  • Proceedings of the National Academy of Sciences, Vol. 108, Issue 37, p. 15248-15252
  • DOI: 10.1073/pnas.1108616108

    Works referencing / citing this record:

    Uranium mobility and accumulation along the Rio Paguate, Jackpile Mine in Laguna Pueblo, NM
    journal, January 2017

    • Blake, Johanna M.; De Vore, Cherie L.; Avasarala, Sumant
    • Environmental Science: Processes & Impacts, Vol. 19, Issue 4
    • DOI: 10.1039/c6em00612d