Search Menu
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information
Search Scholarly Publications

Title: Uranium speciation in acid waste-weathered sediments: The role of aging and phosphate amendments

Abstract

Uranium speciation and lability are strongly coupled to mineral transformations in silicate sediments, particularly for sediments subjected to weathering in acidic, high-level radioactive waste, as occurred at the Department of Energy's Hanford (WA) site. In this study, uncontaminated Hanford sediments were reacted for 365 days with acidic (pH 3), uranium-bearing waste solutions, with and without phosphate in batch experiments, prior to detailed characterizations using electron microscopy, x-ray diffraction and x-ray absorption spectroscopy. In PO4-reactant free systems, uranium speciation was controlled initially by precipitation of compreignacite [K2(UO2)6O4(OH)6·8H2O]- and becquerelite [Ca(UO2)6O4(OH)6·8H2O]-like species. Subsequent further removal of uranium coincided with that of Si and accumulation of boltwoodite, [(K, Na)(UO2)2O4(HSiO4)2•0.5(H2O)]-like species of uranium at 180 and 365 days. When present, PO4 exerted a direct and strong control over U speciation. The detection of meta-ankoleite, [K2(UO2)2O4(PO4)2·6H2O] at all reaction times when U was present emphasizes the importance of dissolved phosphate as a control on U speciation. Here, meta-ankoleite appears well crystallized and when it occurs as the principal product of sediment weathering, its low solubility is expected to limit dissolved U(VI) concentrations in groundwater. Although boltwoodite solubility is also low, it is formed more slowly (and only when PO4 is absent), after initial precipitation ofmore » more soluble, less crystalline uranyl hydroxides. In the context of Hanford crib waste our results suggest that with PO4 present, nearly all uranium would have precipitated in the upper soil.« less

Authors:
 [1];  [2];  [3];  [4];  [3];  [5];  [6];  [7];  [8]
+ Show Author Affiliations
  1. Univ. of Vermont, Burlington, VT (United States). Dept. of Geology
  2. Univ. of Arizona, Tucson, AZ (United States). Dept. of Soil Water and Environmental Science; Univ. of Notre Dame, IN (United States). Dept. of Civil and Environmental Engineering and Earth Sciences
  3. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
  4. Anchor QEA, LLC, Portland, OR (United States)
  5. Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Pohang Univ. of Science and Technology (POSTECH) (Korea, Republic of)
  6. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  7. Univ. of California, Merced, CA (United States). School of Natural Sciences
  8. Univ. of Arizona, Tucson, AZ (United States). Dept. of Soil Water and Environmental Science
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Biological and Environmental Research (BER)
OSTI Identifier:
1413491
Alternate Identifier(s):
OSTI ID: 1476618; OSTI ID: 1548954
Report Number(s):
PNNL-SA-133858
Journal ID: ISSN 0883-2927; PII: S0883292717303657
Grant/Contract Number:  
SBR-DE-SC0006781; AC0576RL01830; AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Applied Geochemistry
Additional Journal Information:
Journal Volume: 89; Journal Issue: C; Journal ID: ISSN 0883-2927
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE WASTES FROM NUCLEAR FACILITIES; uranium; Hanford; acid waste; phosphate; uranyl silicates

Citation Formats

Perdrial, Nicolas, Vázquez-Ortega, Angélica, Wang, Guohui, Kanematsu, Masakazu, Mueller, Karl T., Um, Wooyong, Steefel, Carl I., O'Day, Peggy A., and Chorover, Jon. Uranium speciation in acid waste-weathered sediments: The role of aging and phosphate amendments. United States: N. p., 2017. Web. doi:10.1016/J.APGEOCHEM.2017.12.001.
Copy to clipboard
Perdrial, Nicolas, Vázquez-Ortega, Angélica, Wang, Guohui, Kanematsu, Masakazu, Mueller, Karl T., Um, Wooyong, Steefel, Carl I., O'Day, Peggy A., & Chorover, Jon. Uranium speciation in acid waste-weathered sediments: The role of aging and phosphate amendments. United States. https://doi.org/10.1016/J.APGEOCHEM.2017.12.001
Copy to clipboard
Perdrial, Nicolas, Vázquez-Ortega, Angélica, Wang, Guohui, Kanematsu, Masakazu, Mueller, Karl T., Um, Wooyong, Steefel, Carl I., O'Day, Peggy A., and Chorover, Jon. Tue . "Uranium speciation in acid waste-weathered sediments: The role of aging and phosphate amendments". United States. https://doi.org/10.1016/J.APGEOCHEM.2017.12.001. https://www.osti.gov/servlets/purl/1413491.
Copy to clipboard
@article{osti_1413491,
title = {Uranium speciation in acid waste-weathered sediments: The role of aging and phosphate amendments},
author = {Perdrial, Nicolas and Vázquez-Ortega, Angélica and Wang, Guohui and Kanematsu, Masakazu and Mueller, Karl T. and Um, Wooyong and Steefel, Carl I. and O'Day, Peggy A. and Chorover, Jon},
abstractNote = {Uranium speciation and lability are strongly coupled to mineral transformations in silicate sediments, particularly for sediments subjected to weathering in acidic, high-level radioactive waste, as occurred at the Department of Energy's Hanford (WA) site. In this study, uncontaminated Hanford sediments were reacted for 365 days with acidic (pH 3), uranium-bearing waste solutions, with and without phosphate in batch experiments, prior to detailed characterizations using electron microscopy, x-ray diffraction and x-ray absorption spectroscopy. In PO4-reactant free systems, uranium speciation was controlled initially by precipitation of compreignacite [K2(UO2)6O4(OH)6·8H2O]- and becquerelite [Ca(UO2)6O4(OH)6·8H2O]-like species. Subsequent further removal of uranium coincided with that of Si and accumulation of boltwoodite, [(K, Na)(UO2)2O4(HSiO4)2•0.5(H2O)]-like species of uranium at 180 and 365 days. When present, PO4 exerted a direct and strong control over U speciation. The detection of meta-ankoleite, [K2(UO2)2O4(PO4)2·6H2O] at all reaction times when U was present emphasizes the importance of dissolved phosphate as a control on U speciation. Here, meta-ankoleite appears well crystallized and when it occurs as the principal product of sediment weathering, its low solubility is expected to limit dissolved U(VI) concentrations in groundwater. Although boltwoodite solubility is also low, it is formed more slowly (and only when PO4 is absent), after initial precipitation of more soluble, less crystalline uranyl hydroxides. In the context of Hanford crib waste our results suggest that with PO4 present, nearly all uranium would have precipitated in the upper soil.},
doi = {10.1016/J.APGEOCHEM.2017.12.001},
journal = {Applied Geochemistry},
number = C,
volume = 89,
place = {United States},
year = {Tue Dec 05 00:00:00 EST 2017},
month = {Tue Dec 05 00:00:00 EST 2017}
}
Copy to clipboard
Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1016/J.APGEOCHEM.2017.12.001
Copyright Statement
Other availability
Search WorldCat Search WorldCat to find libraries that may hold this journal
Citation Metrics:
Cited by: 12 works
Citation information provided by
Web of Science

Figures / Tables:

Figure 1 Figure 1: Evolution of solution chemistry during reaction for pH (a), Total inorganic carbon reported as CO32- (b), U (c), total PO43- (note the break on the y-axis) (d), Si (e) and Mg (f). Note the y-axis break for panel d.
All figures and tables (9 total)
Save / Share:
Export Metadata
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.

Works referenced in this record:

Impact of highly basic solutions on sorption of Cs+ to subsurface sediments from the Hanford site, USA
journal, October 2005

  • Ainsworth, C. C.; Zachara, J. M.; Wagnon, K.
  • Geochimica et Cosmochimica Acta, Vol. 69, Issue 20
  • DOI: 10.1016/j.gca.2005.06.007

The aqueous chemistry of uranium minerals. Part 2. Minerals of the liebigite group
journal, March 1980

Spectroscopic Evidence for Uranium Bearing Precipitates in Vadose Zone Sediments at the Hanford 300-Area Site
journal, July 2007

  • Arai, Yuji; Marcus, M. A.; Tamura, N.
  • Environmental Science & Technology, Vol. 41, Issue 13
  • DOI: 10.1021/es062196u

Evaluation of an Acid Ammonium Oxalate Extraction to Determine Fluoride Resident Concentrations in Soils
journal, March 2003

  • Bégin, Louis; Fortin, Josée
  • Journal of Environmental Quality, Vol. 32, Issue 2
  • DOI: 10.2134/jeq2003.6620

Nitrate-Cancrinite Precipitation on Quartz Sand in Simulated Hanford Tank Solutions
journal, November 2001

  • Bickmore, Barry R.; Nagy, Kathryn L.; Young, James S.
  • Environmental Science & Technology, Vol. 35, Issue 22
  • DOI: 10.1021/es0108234

Mineralization of contaminant uranium and leach rates in sediments from Hanford, Washington
journal, January 2010

The surface chemistry of dissolving labradorite feldspar
journal, April 1989

  • Casey, William H.; Westrich, Henry R.; Arnold, George W.
  • Geochimica et Cosmochimica Acta, Vol. 53, Issue 4
  • DOI: 10.1016/0016-7037(89)90028-8

Spectroscopic and Diffraction Study of Uranium Speciation in Contaminated Vadose Zone Sediments from the Hanford Site, Washington State
journal, May 2004

  • Catalano, Jeffrey G.; Heald, Steven M.; Zachara, John M.
  • Environmental Science & Technology, Vol. 38, Issue 10
  • DOI: 10.1021/es049963e

Changes in Uranium Speciation through a Depth Sequence of Contaminated Hanford Sediments
journal, April 2006

  • Catalano, Jeffrey G.; McKinley, James P.; Zachara, John M.
  • Environmental Science & Technology, Vol. 40, Issue 8
  • DOI: 10.1021/es0520969

Strontium and Cesium Release Mechanisms during Unsaturated Flow through Waste-Weathered Hanford Sediments
journal, October 2011

  • Chang, Hyun-shik; Um, Wooyong; Rod, Kenton
  • Environmental Science & Technology, Vol. 45, Issue 19
  • DOI: 10.1021/es2010368

The Gibbs free energies and enthalpies of formation of U (super 6+) phases; an empirical method of prediction
journal, April 1999

  • Chen, Fanrong; Ewing, Rodney C.; Clark, Sue B.
  • American Mineralogist, Vol. 84, Issue 4
  • DOI: 10.2138/am-1999-0418

Silicon control of strontium and cesium partitioning in hydroxide-weathered sediments
journal, April 2008

  • Chorover, Jon; Choi, Sunkyung; Rotenberg, Paula
  • Geochimica et Cosmochimica Acta, Vol. 72, Issue 8
  • DOI: 10.1016/j.gca.2008.01.026

Uranium co-precipitation with iron oxide minerals
journal, October 2002

  • Duff, Martine C.; Coughlin, Jessica Urbanik; Hunter, Douglas B.
  • Geochimica et Cosmochimica Acta, Vol. 66, Issue 20
  • DOI: 10.1016/S0016-7037(02)00953-5

Orthoclase dissolution kinetics probed by in situ X-ray reflectivity: effects of temperature, pH, and crystal orientation
journal, January 2003

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

Uranium fate in Hanford sediment altered by simulated acid waste solutions
journal, December 2015

Solubility measurements of the uranyl oxide hydrate phases metaschoepite, compreignacite, Na–compreignacite, becquerelite, and clarkeite
journal, June 2008

  • Gorman-Lewis, Drew; Fein, Jeremy B.; Burns, Peter C.
  • The Journal of Chemical Thermodynamics, Vol. 40, Issue 6
  • DOI: 10.1016/j.jct.2008.02.006

Crystallography Open Database – an open-access collection of crystal structures
journal, May 2009

  • Gražulis, Saulius; Chateigner, Daniel; Downs, Robert T.
  • Journal of Applied Crystallography, Vol. 42, Issue 4
  • DOI: 10.1107/S0021889809016690

Crystallography Open Database (COD): an open-access collection of crystal structures and platform for world-wide collaboration
journal, November 2011

  • Gražulis, Saulius; Daškevič, Adriana; Merkys, Andrius
  • Nucleic Acids Research, Vol. 40, Issue D1
  • DOI: 10.1093/nar/gkr900

The albite-water system: Part IV. Diffusion modeling of leached and hydrogen-enriched layers
journal, April 1997

The complexity of mineral dissolution as viewed by high resolution scanning Auger microscopy: Labradorite under hydrothermal conditions
journal, February 1988

Influence of Phosphate and Silica on U(VI) Precipitation from Acidic and Neutralized Wastewaters
journal, May 2014

  • Kanematsu, Masakazu; Perdrial, Nicolas; Um, Wooyong
  • Environmental Science & Technology, Vol. 48, Issue 11
  • DOI: 10.1021/es4056559

Environmental Speciation of Actinides
journal, June 2012

  • Maher, Kate; Bargar, John R.; Brown, Gordon E.
  • Inorganic Chemistry, Vol. 52, Issue 7
  • DOI: 10.1021/ic301686d

Silica- and sulfate-bearing rock coatings in smelter areas: Products of chemical weathering and atmospheric pollution I. Formation and mineralogical composition
journal, May 2012

  • Mantha, Nathalie M.; Schindler, Michael; Murayama, Mitsuhiro
  • Geochimica et Cosmochimica Acta, Vol. 85
  • DOI: 10.1016/j.gca.2012.01.033

Colloid Formation in Hanford Sediments Reacted with Simulated Tank Waste
journal, November 2004

  • Mashal, Kholoud; Harsh, James B.; Flury, Markus
  • Environmental Science & Technology, Vol. 38, Issue 21
  • DOI: 10.1021/es0349709

DITHIONITE- AND OXALATE-EXTRACTABLE Fe AND Al AS AIDS IN DIFFERENTIATING VARIOUS CLASSES OF SOILS
journal, February 1966

  • McKeague, J. A.; Day, J. H.
  • Canadian Journal of Soil Science, Vol. 46, Issue 1
  • DOI: 10.4141/cjss66-003

Geochemical Controls on Contaminant Uranium in Vadose Hanford Formation Sediments at the 200 Area and 300 Area, Hanford Site, Washington
journal, January 2007

  • McKinley, James P.; Zachara, John M.; Wan, Jiamin
  • Vadose Zone Journal, Vol. 6, Issue 4
  • DOI: 10.2136/vzj2006.0184

Effect of co-solutes on the products and solubility of uranium(VI) precipitated with phosphate
journal, January 2014

Field evidence for uranium nanocrystallization and its implications for uranium transport
journal, September 2005

The surface chemistry of multi-oxide silicates
journal, August 2009

  • Oelkers, Eric H.; Golubev, Sergey V.; Chairat, Claire
  • Geochimica et Cosmochimica Acta, Vol. 73, Issue 16
  • DOI: 10.1016/j.gca.2009.05.028

Phosphate-Induced Immobilization of Uranium in Hanford Sediments
journal, November 2016

  • Pan, Zezhen; Giammar, Daniel E.; Mehta, Vrajesh
  • Environmental Science & Technology, Vol. 50, Issue 24
  • DOI: 10.1021/acs.est.6b02928

Trace contaminant concentration affects mineral transformation and pollutant fate in hydroxide-weathered Hanford sediments
journal, December 2011

Mineral transformation controls speciation and pore-fluid transmission of contaminants in waste-weathered Hanford sediments
journal, September 2014

  • Perdrial, Nicolas; Thompson, Aaron; O’Day, Peggy A.
  • Geochimica et Cosmochimica Acta, Vol. 141
  • DOI: 10.1016/j.gca.2014.06.022

Thermodynamics of aragonite-strontianite solid solutions: Results from stoichiometric solubility at 25 and 76°C
journal, June 1987

Transport-controlled kinetics of dissolution and precipitation in the sediments under alkaline and saline conditions
journal, July 2004

  • Qafoku, Nikolla P.; Ainsworth, Calvin C.; Szecsody, James E.
  • Geochimica et Cosmochimica Acta, Vol. 68, Issue 14
  • DOI: 10.1016/j.gca.2003.12.017

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

Rates and mechanisms of uranyl oxyhydroxide mineral dissolution
journal, June 2017

  • Reinoso-Maset, Estela; Steefel, Carl I.; Um, Wooyong
  • Geochimica et Cosmochimica Acta, Vol. 207
  • DOI: 10.1016/j.gca.2017.03.009

Transport of Strontium and Cesium in Simulated Hanford Tank Waste Leachate through Quartz Sand under Saturated and Unsaturated Flow
journal, November 2010

  • Rod, Kenton A.; Um, Wooyong; Flury, Markus
  • Environmental Science & Technology, Vol. 44, Issue 21
  • DOI: 10.1021/es903223x

Diffusive release of uranium from contaminated sediments into capillary fringe pore water
journal, October 2012

Near-surface composition of acid-leached labradorite investigated by SIMS
journal, May 1997

Uranium Speciation As a Function of Depth in Contaminated Hanford Sediments - A Micro-XRF, Micro-XRD, and Micro- And Bulk-XAFS Study
journal, February 2009

  • Singer, David M.; Zachara, John M.; Brown Jr, Gordon E.
  • Environmental Science & Technology, Vol. 43, Issue 3
  • DOI: 10.1021/es8021045

Newly recognized hosts for uranium in the Hanford Site vadose zone
journal, March 2009

  • Stubbs, Joanne E.; Veblen, Linda A.; Elbert, David C.
  • Geochimica et Cosmochimica Acta, Vol. 73, Issue 6
  • DOI: 10.1016/j.gca.2008.12.004

Prediction of Aluminum, Uranium, and Co-Contaminants Precipitation and Adsorption during Titration of Acidic Sediments
journal, May 2013

  • Tang, Guoping; Luo, Wensui; Watson, David B.
  • Environmental Science & Technology, Vol. 47, Issue 11
  • DOI: 10.1021/es400169y

Contaminant Desorption during Long-Term Leaching of Hydroxide-Weathered Hanford Sediments
journal, March 2010

  • Thompson, Aaron; Steefel, Carl I.; Perdrial, Nicolas
  • Environmental Science & Technology, Vol. 44, Issue 6
  • DOI: 10.1021/es902043e

Characterization of uranium-contaminated sediments from beneath a nuclear waste storage tank from Hanford, Washington: Implications for contaminant transport and fate
journal, February 2010

  • Um, Wooyong; Icenhower, Jonathan P.; Brown, Christopher F.
  • Geochimica et Cosmochimica Acta, Vol. 74, Issue 4
  • DOI: 10.1016/j.gca.2009.11.014

Uranium Phases in Contaminated Sediments below Hanford’s U Tank Farm
journal, May 2009

  • Um, Wooyong; Wang, Zheming; Serne, R. Jeffrey
  • Environmental Science & Technology, Vol. 43, Issue 12
  • DOI: 10.1021/es900203r

Geochemical evolution of highly alkaline and saline tank waste plumes during seepage through vadose zone sediments
journal, February 2004

Efficacy of soluble sodium tripolyphosphate amendments for the in-situ immobilisation of uranium
journal, January 2007

  • Wellman, Dawn M.; Pierce, Eric M.; Valenta, Michelle M.
  • Environmental Chemistry, Vol. 4, Issue 5
  • DOI: 10.1071/EN07030

Sequestration and retention of uranium(VI) in the presence of hydroxylapatite under dynamic geochemical conditions
journal, January 2008

  • Wellman, Dawn M.; Glovack, Julia N.; Parker, Kent
  • Environmental Chemistry, Vol. 5, Issue 1
  • DOI: 10.1071/EN07060

Uranium release and secondary phase formation during unsaturated testing of UO2 at 90°C
journal, August 1992

Geochemical Processes Controlling Migration of Tank Wastes in Hanford's Vadose Zone
journal, January 2007

  • Zachara, John M.; Serne, Jeff; Freshley, Mark
  • Vadose Zone Journal, Vol. 6, Issue 4
  • DOI: 10.2136/vzj2006.0180

Extraction of Oxidized and Reduced Forms of Uranium from Contaminated Soils:  Effects of Carbonate Concentration and pH
journal, June 2005

  • Zhou, Ping; Gu, Baohua
  • Environmental Science & Technology, Vol. 39, Issue 12
  • DOI: 10.1021/es0483443
    Sort by:
    [ × clear filter / sort ]

    Works referencing / citing this record:

      Sort by:
      [ × clear filter / sort ]

      Figures / Tables found in this record:

      Figure 1 (p. 19)figure
      Figure 2 (p. 21)figure
      Table 1 (p. 21)table
      Figure 3 (p. 22)figure
      Figure 4 (p. 23)figure
      Figure 5 (p. 24)figure
      Table 2 (p. 25)table
      Figure 6 (p. 28)figure
      Figure 7 (p. 30)figure
        [ × clear filter / sort ]
        Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.

        Similar Records in DOE PAGES and OSTI.GOV collections: