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Title: Dynamic interplay between uranyl phosphate precipitation, sorption, and phase evolution

Abstract

We report that natural examples demonstrate uranyl-phosphate minerals can maintain extremely low levels of aqueous uranium in groundwaters due to their low solubility. Thus, greater understanding of the geochemical factors leading to uranyl phosphate precipitation may lead to successful application of phosphate-based remediation methods. However, the solubility of uranyl phosphate phases varies over >3 orders of magnitude, with the most soluble phases typically observed in lab experiments. To understand the role of common soil/sediment mineral surfaces in the nucleation and transformation of uranyl phosphate minerals under environmentally relevant conditions, we carried out batch experiments with goethite and mica at pH 6 in mixed electrolyte solutions ranging from 1–800 μM U and 1–800 μM P. All experiments ended with uranium concentrations below the USEPA MCL for U, but with 2–3 orders of magnitude difference in uranium concentrations.

Authors:
 [1];  [1];  [2];  [1]
  1. Univ. of Oklahoma, Norman, OK (United States). School of Geology and Geophysics
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Environmental Sciences Division
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1265483
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Applied Geochemistry
Additional Journal Information:
Journal Volume: 58; Journal Issue: C; Journal ID: ISSN 0883-2927
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
58 GEOSCIENCES; 54 ENVIRONMENTAL SCIENCES

Citation Formats

Munasinghe, P. Sumudu, Elwood Madden, Megan E., Brooks, Scott C., and Elwood Madden, Andrew S. Dynamic interplay between uranyl phosphate precipitation, sorption, and phase evolution. United States: N. p., 2015. Web. doi:10.1016/j.apgeochem.2015.04.008.
Munasinghe, P. Sumudu, Elwood Madden, Megan E., Brooks, Scott C., & Elwood Madden, Andrew S. Dynamic interplay between uranyl phosphate precipitation, sorption, and phase evolution. United States. https://doi.org/10.1016/j.apgeochem.2015.04.008
Munasinghe, P. Sumudu, Elwood Madden, Megan E., Brooks, Scott C., and Elwood Madden, Andrew S. Fri . "Dynamic interplay between uranyl phosphate precipitation, sorption, and phase evolution". United States. https://doi.org/10.1016/j.apgeochem.2015.04.008. https://www.osti.gov/servlets/purl/1265483.
@article{osti_1265483,
title = {Dynamic interplay between uranyl phosphate precipitation, sorption, and phase evolution},
author = {Munasinghe, P. Sumudu and Elwood Madden, Megan E. and Brooks, Scott C. and Elwood Madden, Andrew S.},
abstractNote = {We report that natural examples demonstrate uranyl-phosphate minerals can maintain extremely low levels of aqueous uranium in groundwaters due to their low solubility. Thus, greater understanding of the geochemical factors leading to uranyl phosphate precipitation may lead to successful application of phosphate-based remediation methods. However, the solubility of uranyl phosphate phases varies over >3 orders of magnitude, with the most soluble phases typically observed in lab experiments. To understand the role of common soil/sediment mineral surfaces in the nucleation and transformation of uranyl phosphate minerals under environmentally relevant conditions, we carried out batch experiments with goethite and mica at pH 6 in mixed electrolyte solutions ranging from 1–800 μM U and 1–800 μM P. All experiments ended with uranium concentrations below the USEPA MCL for U, but with 2–3 orders of magnitude difference in uranium concentrations.},
doi = {10.1016/j.apgeochem.2015.04.008},
journal = {Applied Geochemistry},
number = C,
volume = 58,
place = {United States},
year = {Fri Apr 17 00:00:00 EDT 2015},
month = {Fri Apr 17 00:00:00 EDT 2015}
}

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Cited by: 19 works
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Works referenced in this record:

Immobilization of Uranium in Contaminated Sediments by Hydroxyapatite Addition
journal, December 1998

  • Arey, J. Samuel; Seaman, John C.; Bertsch, Paul M.
  • Environmental Science & Technology, Vol. 33, Issue 2
  • DOI: 10.1021/es980425+

Effect of sulfate, carbonate, and phosphate on the uranium(VI) sorption behavior onto bentonite
journal, January 2008

  • Bachmaf, Samer; Planer-Friedrich, Britta; Merkel, Broder J.
  • Radiochimica Acta, Vol. 96, Issue 6
  • DOI: 10.1524/ract.2008.1496

Nonreductive Biomineralization of Uranium(VI) Phosphate Via Microbial Phosphatase Activity in Anaerobic Conditions
journal, September 2009

  • Beazley, Melanie J.; Martinez, Robert J.; Sobecky, Patricia A.
  • Geomicrobiology Journal, Vol. 26, Issue 7
  • DOI: 10.1080/01490450903060780

The effect of pH and natural microbial phosphatase activity on the speciation of uranium in subsurface soils
journal, October 2011

  • Beazley, Melanie J.; Martinez, Robert J.; Webb, Samuel M.
  • Geochimica et Cosmochimica Acta, Vol. 75, Issue 19
  • DOI: 10.1016/j.gca.2011.07.006

Uranyl Surface Complexes Formed on Subsurface Media from DOE Facilities
journal, January 2002

  • Bostick, Benjamin C.; Fendorf, Scott; Barnett, Mark O.
  • Soil Science Society of America Journal, Vol. 66, Issue 1
  • DOI: 10.2136/sssaj2002.0099

Contaminant Uranium Phases and Leaching at the Fernald Site in Ohio
journal, January 1996

  • Buck, Edgar C.; Brown, Neil R.; Dietz, Nancy L.
  • Environmental Science & Technology, Vol. 30, Issue 1
  • DOI: 10.1021/es9500825

Oxidative Dissolution of Biogenic Uraninite in Groundwater at Old Rifle, CO
journal, October 2011

  • Campbell, Kate M.; Veeramani, Harish; Ulrich, Kai-Uwe
  • Environmental Science & Technology, Vol. 45, Issue 20
  • DOI: 10.1021/es200482f

Uranyl adsorption onto montmorillonite: Evaluation of binding sites and carbonate complexation
journal, June 2005


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

Effects of Phosphate on Uranium(VI) Adsorption to Goethite-Coated Sand
journal, November 2004

  • Cheng, Tao; Barnett, Mark O.; Roden, Eric E.
  • Environmental Science & Technology, Vol. 38, Issue 22
  • DOI: 10.1021/es040388o

Reactive transport of uranium(VI) and phosphate in a goethite-coated sand column: An experimental study
journal, July 2007


Confocal Micrometer-Scale X-ray Fluorescence and X-ray Absorption Fine Structure Studies of Uranium Speciation in a Tertiary Sediment from a Waste Disposal Natural Analogue Site
journal, April 2005

  • Denecke, Melissa A.; Janssens, Koen; Proost, Kristof
  • Environmental Science & Technology, Vol. 39, Issue 7
  • DOI: 10.1021/es048644k

The solubility product of NaUO 2 PO 4 · x H 2 O determined in phosphate and carbonate solutions
journal, July 2005


Remediation of Soils and Wastes Contaminated with Uranium and Toxic Metals
journal, December 1998

  • Francis, A. J.; Dodge, C. J.
  • Environmental Science & Technology, Vol. 32, Issue 24
  • DOI: 10.1021/es9803310

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

Time Scales for Sorption−Desorption and Surface Precipitation of Uranyl on Goethite
journal, August 2001

  • Giammar, Daniel E.; Hering, Janet G.
  • Environmental Science & Technology, Vol. 35, Issue 16
  • DOI: 10.1021/es0019981

Review of uranyl mineral solubility measurements
journal, March 2008

  • Gorman-Lewis, Drew; Burns, Peter C.; Fein, Jeremy B.
  • The Journal of Chemical Thermodynamics, Vol. 40, Issue 3
  • DOI: 10.1016/j.jct.2007.12.004

Thermodynamic Properties of Autunite, Uranyl Hydrogen Phosphate, and Uranyl Orthophosphate from Solubility and Calorimetric Measurements
journal, October 2009

  • Gorman-Lewis, Drew; Shvareva, Tatiana; Kubatko, Karrie-Ann
  • Environmental Science & Technology, Vol. 43, Issue 19
  • DOI: 10.1021/es9012933

Sorption of U(VI) and phosphate on γ-alumina: Binary and ternary sorption systems
journal, March 2009

  • Guo, Zhijun; Yan, Chao; Xu, Jiang
  • Colloids and Surfaces A: Physicochemical and Engineering Aspects, Vol. 336, Issue 1-3
  • DOI: 10.1016/j.colsurfa.2008.11.032

U 6+ phases in the weathering zone of the Bangombé U-deposit: observed and predicted mineralogy
journal, September 2002


Geochemical coupling of uranium and phosphorous in soils overlying an unmined uranium deposit: Coles Hill, Virginia
journal, October 2006


Phosphate based immobilization of uranium in an oxidizing bedrock aquifer
journal, June 2003


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

Sorption mechanism of U(VI) on a reference montmorillonite: Binding to the internal and external surfaces
journal, January 2001

  • Kim, S. J.
  • Journal of Radioanalytical and Nuclear Chemistry, Vol. 250, Issue 1, p. 55-62
  • DOI: 10.1023/A:1013212130177

Uranium solution-mineral equilibria at low temperatures with applications to sedimentary ore deposits
journal, June 1978


The crystal structure of synthetic autunite, Ca[(UO 2 )(PO 4 )] 2 (H 2 O) 11
journal, January 2003

  • Locock, Andrew J.; Burns, Peter C.
  • American Mineralogist, Vol. 88, Issue 1
  • DOI: 10.2138/am-2003-0128

Aqueous Pb sorption by hydroxylapatite; applications of atomic force microscopy to dissolution, nucleation, and growth studies
journal, February 1998

  • Lower, Steven K.; Maurice, Patricia A.; Traina, Samuel J.
  • American Mineralogist, Vol. 83, Issue 1-2
  • DOI: 10.2138/am-1998-1-215

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


Speciation of Uranium in Fernald Soils by Molecular Spectroscopic Methods:  Characterization of Untreated Soils
journal, January 1996

  • Morris, David E.; Allen, Patrick G.; Berg, John M.
  • Environmental Science & Technology, Vol. 30, Issue 7
  • DOI: 10.1021/es950745i

Mobility of uranium during weathering
journal, October 1997

  • Murakami, Takashi; Ohnuki, Toshihiko; Isobe, Hiroshi
  • American Mineralogist, Vol. 82, Issue 9-10
  • DOI: 10.2138/am-1997-9-1006

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


The biogeochemistry and bioremediation of uranium and other priority radionuclides
journal, January 2014


In situ TEM imaging of CaCO3 nucleation reveals coexistence of direct and indirect pathways
journal, September 2014


Uranium(6+) sorption on montmorillonite: Experimental and surface complexation modeling study
journal, September 1996

  • Pabalan, Roberto T.; Turner, David R.
  • Aquatic Geochemistry, Vol. 2, Issue 3
  • DOI: 10.1007/BF01160043

Phosphate Fixation by Soil Minerals: Mica and Related Groups
journal, January 1944


Distribution of Uranium Contamination in Weathered Fractured Saprolite/Shale and Ground Water
journal, September 2006

  • Phillips, D. H.; Watson, D. B.; Roh, Y.
  • Journal of Environmental Quality, Vol. 35, Issue 5
  • DOI: 10.2134/jeq2005.0124

Solubility of (UO2)3(PO4)2⋅4H2O in H+-Na+-OH−-H2PO−4-HPO2−4-PO3−4-H2O and Its Comparison to the Analogous PuO2 +2 System
journal, April 2005


Physicochemical and Mineralogical Characterization of Uranium-Contaminated Soils
journal, September 2000


Surface complexation modeling of the effects of phosphate on uranium(VI) adsorption
journal, May 2007


Inhibition Effect of Secondary Phosphate Mineral Precipitation on Uranium Release from Contaminated Sediments
journal, November 2009

  • Shi, Zhenqing; Liu, Chongxuan; Zachara, John M.
  • Environmental Science & Technology, Vol. 43, Issue 21
  • DOI: 10.1021/es9021359

Impact of phosphate on U(VI) immobilization in the presence of goethite
journal, November 2010

  • Singh, Abhas; Ulrich, Kai-Uwe; Giammar, Daniel E.
  • Geochimica et Cosmochimica Acta, Vol. 74, Issue 22
  • DOI: 10.1016/j.gca.2010.08.031

Molecular-Scale Structure of Uranium(VI) Immobilized with Goethite and Phosphate
journal, May 2012

  • Singh, Abhas; Catalano, Jeffrey G.; Ulrich, Kai-Uwe
  • Environmental Science & Technology, Vol. 46, Issue 12
  • DOI: 10.1021/es300494x

A new kinetic approach to modeling water-rock interaction: The role of nucleation, precursors, and Ostwald ripening
journal, October 1990


Modelling the adsorption of uranyl on the surface of goethite
journal, April 2002


Electron Microbeam Investigation of Uranium-Contaminated Soils from Oak Ridge, TN, USA
journal, April 2006

  • Stubbs, Joanne E.; Elbert, David C.; Veblen, David R.
  • Environmental Science & Technology, Vol. 40, Issue 7
  • DOI: 10.1021/es0518676

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

Competitive Sorption of Arsenate and Phosphate on Different Clay Minerals and Soils
journal, January 2002

  • Violante, Antonio; Pigna, Massimo
  • Soil Science Society of America Journal, Vol. 66, Issue 6
  • DOI: 10.2136/sssaj2002.1788

Calcium Orthophosphates: Crystallization and Dissolution
journal, November 2008

  • Wang, Lijun; Nancollas, George H.
  • Chemical Reviews, Vol. 108, Issue 11
  • DOI: 10.1021/cr0782574

Effects of pH, temperature, and aqueous organic material on the dissolution kinetics of meta-autunite minerals, (Na, Ca) 2−1 [(UO 2 )(PO 4 )] 2 · 3H 2 O
journal, January 2006

  • Wellman, Dawn M.; Icenhower, Jonathan P.; Gamerdinger, Amy P.
  • American Mineralogist, Vol. 91, Issue 1
  • DOI: 10.2138/am.2006.1807

Comparative Analysis of Soluble Phosphate Amendments for the Remediation of Heavy Metal Contaminants: Effect on Sediment Hydraulic Conductivity
journal, January 2006

  • Wellman, Dawn M.; Icenhower, Jonathan P.; Owen, Antoinette T.
  • Environmental Chemistry, Vol. 3, Issue 3
  • DOI: 10.1071/EN05023

Dissolution kinetics of meta-torbernite under circum-neutral to alkaline conditions
journal, January 2009

  • Wellman, Dawn M.; McNamara, Bruce K.; Bacon, Diana H.
  • Environmental Chemistry, Vol. 6, Issue 6
  • DOI: 10.1071/EN09046

Evaluation of the Efficacy of Polyphosphate Remediation Technology: Direct and Indirect Remediation of Uranium Under Alkaline Conditions
journal, February 2011


Sodium meta-autunite colloids: Synthesis, characterization, and stability
journal, February 2006

  • Zheng, Zuoping; Wan, Jiamin; Song, Xiangyun
  • Colloids and Surfaces A: Physicochemical and Engineering Aspects, Vol. 274, Issue 1-3
  • DOI: 10.1016/j.colsurfa.2005.08.032

Works referencing / citing this record:

Uranium speciation in weathered granitic waste rock piles: an XAFS investigation
journal, January 2019

  • Tayal, Akhil; Conradson, Steven D.; Kanzari, Aisha
  • RSC Advances, Vol. 9, Issue 21
  • DOI: 10.1039/c9ra00961b

Biogeochemical Modelling of Uranium Immobilization and Aquifer Remediation Strategies Near NCCP Sludge Storage Facilities
journal, March 2021

  • Safonov, Alexey V.; Boguslavsky, Anatoly E.; Gaskova, Olga L.
  • Applied Sciences, Vol. 11, Issue 6
  • DOI: 10.3390/app11062875