Phosphate-Induced Immobilization of Uranium in Hanford Sediments

Pan, Zezhen; Giammar, Daniel E.; Mehta, Vrajesh; Troyer, Lyndsay D.; Catalano, Jeffrey G.; Wang, Zheming

doi:10.1021/acs.est.6b02928

Title: Phosphate-Induced Immobilization of Uranium in Hanford Sediments

Journal Article · Tue Nov 29 00:00:00 EST 2016 · Environmental Science and Technology

DOI:https://doi.org/10.1021/acs.est.6b02928· OSTI ID:1346213

Pan, Zezhen ^[1];

^[1]; Mehta, Vrajesh ^[1]; Troyer, Lyndsay D. ^[1];

^[1]; Wang, Zheming ^[2]

Washington Univ., St. Louis, MO (United States)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

Phosphate can be added to subsurface environments to immobilize U(VI) contamination. The efficacy of immobilization depends on the site-specific groundwater chemistry and aquifer sediment properties. Batch and column experiments were performed with sediments from the Hanford 300 Area in Washington State and artificial groundwater prepared to emulate the conditions at the site. These experiments quantified the effect of phosphate on U(VI) transport and suggested dominant immobilization reactions. Batch experiments revealed enhanced U(VI) sorption with increasing phosphate addition. X-ray absorption spectroscopy measurements of samples from the batch experiments observed U(VI) phosphate precipitates only at high initial U(VI) and phosphate loadings and found that U(VI) was predominantly adsorbed at the most environmentally relevant conditions. In column experiments more U(VI) was retained in sediments when phosphate-containing groundwater was introduced to U(VI)-loaded sediments than when the groundwater did not contain phosphate. The benefits of phosphate addition for U(VI) immobilization persisted for one month even after phosphate addition was stopped. Sequential extractions and laser-induced fluorescence spectroscopy of sediments from the columns suggested that the retained U(VI) was primarily in adsorbed forms.

View Accepted Manuscript (DOE)

Cite

Export

Save

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Biological and Environmental Research (BER)

Grant/Contract Number:: AC02-06CH11357; SC0006857; AC05-76RL01830

OSTI ID:: 1346213

Alternate ID(s):: OSTI ID: 1755205

Report Number(s):: PNNL-SA-121196

Journal Information:: Environmental Science and Technology, Vol. 50, Issue 24; ISSN 0013-936X

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: ENGLISH

Citation Metrics:

Cited by: 32 works

Citation information provided by
Web of Science

References (39)

Phosphate based immobilization of uranium in an oxidizing bedrock aquifer Jerden, James L.; Sinha, A. K. Applied Geochemistry, Vol. 18, Issue 6 https://doi.org/10.1016/S0883-2927(02)00179-8	journal	June 2003
Mechanisms of Uranium Interactions with Hydroxyapatite: Implications for Groundwater Remediation Fuller, C. C.; Bargar, J. R.; Davis, J. A. Environmental Science & Technology, Vol. 36, Issue 2 https://doi.org/10.1021/es0108483	journal	January 2002
Inhibition Effect of Secondary Phosphate Mineral Precipitation on Uranium Release from Contaminated Sediments Shi, Zhenqing; Liu, Chongxuan; Zachara, John M. Environmental Science & Technology, Vol. 43, Issue 21 https://doi.org/10.1021/es9021359	journal	November 2009
Effect of Reaction Pathway on the Extent and Mechanism of Uranium(VI) Immobilization with Calcium and Phosphate Mehta, Vrajesh S.; Maillot, Fabien; Wang, Zheming Environmental Science & Technology, Vol. 50, Issue 6 https://doi.org/10.1021/acs.est.5b06212	journal	February 2016
Effect of co-solutes on the products and solubility of uranium(VI) precipitated with phosphate Mehta, Vrajesh S.; Maillot, Fabien; Wang, Zheming Chemical Geology, Vol. 364 https://doi.org/10.1016/j.chemgeo.2013.12.002	journal	January 2014
Influence of Phosphate and Silica on U(VI) Precipitation from Acidic and Neutralized Wastewaters Kanematsu, Masakazu; Perdrial, Nicolas; Um, Wooyong Environmental Science & Technology, Vol. 48, Issue 11 https://doi.org/10.1021/es4056559	journal	May 2014
Impact of phosphate on U(VI) immobilization in the presence of goethite Singh, Abhas; Ulrich, Kai-Uwe; Giammar, Daniel E. Geochimica et Cosmochimica Acta, Vol. 74, Issue 22 https://doi.org/10.1016/j.gca.2010.08.031	journal	November 2010
Molecular-Scale Structure of Uranium(VI) Immobilized with Goethite and Phosphate Singh, Abhas; Catalano, Jeffrey G.; Ulrich, Kai-Uwe Environmental Science & Technology, Vol. 46, Issue 12 https://doi.org/10.1021/es300494x	journal	May 2012
Effects of Phosphate on Uranium(VI) Adsorption to Goethite-Coated Sand Cheng, Tao; Barnett, Mark O.; Roden, Eric E. Environmental Science & Technology, Vol. 38, Issue 22 https://doi.org/10.1021/es040388o	journal	November 2004
Changes in Uranium Speciation through a Depth Sequence of Contaminated Hanford Sediments Catalano, Jeffrey G.; McKinley, James P.; Zachara, John M. Environmental Science & Technology, Vol. 40, Issue 8 https://doi.org/10.1021/es0520969	journal	April 2006
Characterizing particle-scale equilibrium adsorption and kinetics of uranium(VI) desorption from U-contaminated sediments: RELATING URANIUM MASS-TRANSFER RATES TO MICROPOROSITY Stoliker, Deborah L.; Liu, Chongxuan; Kent, Douglas B. Water Resources Research, Vol. 49, Issue 2 https://doi.org/10.1002/wrcr.20104	journal	February 2013
Kinetic Desorption and Sorption of U(VI) during Reactive Transport in a Contaminated Hanford Sediment Qafoku, Nikolla P.; Zachara, John M.; Liu, Chongxuan Environmental Science & Technology, Vol. 39, Issue 9 https://doi.org/10.1021/es048462q	journal	May 2005
Uranium Speciation As a Function of Depth in Contaminated Hanford Sediments - A Micro-XRF, Micro-XRD, and Micro- And Bulk-XAFS Study Singer, David M.; Zachara, John M.; Brown Jr, Gordon E. Environmental Science & Technology, Vol. 43, Issue 3 https://doi.org/10.1021/es8021045	journal	February 2009
Spectroscopic Evidence for Uranium Bearing Precipitates in Vadose Zone Sediments at the Hanford 300-Area Site Arai, Yuji; Marcus, M. A.; Tamura, N. Environmental Science & Technology, Vol. 41, Issue 13 https://doi.org/10.1021/es062196u	journal	July 2007
Adsorption and Transport of Uranium(VI) in Subsurface Media Barnett, M. O.; Jardine, P. M.; Brooks, S. C. Soil Science Society of America Journal, Vol. 64, Issue 3 https://doi.org/10.2136/sssaj2000.643908x	journal	January 2000
300 Area Uranium Leach and Adsorption Project Serne, R. Jeffrey; Brown, Christopher F.; Schaef, Herbert T. https://doi.org/10.2172/15010052	report	November 2002
Quantifying Differences in the Impact of Variable Chemistry on Equilibrium Uranium(VI) Adsorption Properties of Aquifer Sediments Stoliker, Deborah L.; Kent, Douglas B.; Zachara, John M. Environmental Science & Technology, Vol. 45, Issue 20 https://doi.org/10.1021/es202677v	journal	October 2011
300 Area Uranium Stabilization Through Polyphosphate Injection: Final Report Vermeul, Vincent R.; Bjornstad, Bruce N.; Fritz, Brad G. https://doi.org/10.2172/967237	report	June 2009
Transport of U(VI) through sediments amended with phosphate to induce in situ uranium immobilization Mehta, Vrajesh S.; Maillot, Fabien; Wang, Zheming Water Research, Vol. 69 https://doi.org/10.1016/j.watres.2014.11.044	journal	February 2015
Persistence of uranium groundwater plumes: Contrasting mechanisms at two DOE sites in the groundwater–river interaction zone Zachara, John M.; Long, Philip E.; Bargar, John Journal of Contaminant Hydrology, Vol. 147 https://doi.org/10.1016/j.jconhyd.2013.02.001	journal	April 2013
Geochemical, mineralogical and microbiological characteristics of sediment from a naturally reduced zone in a uranium-contaminated aquifer Campbell, K. M.; Kukkadapu, R. K.; Qafoku, N. P. Applied Geochemistry, Vol. 27, Issue 8 https://doi.org/10.1016/j.apgeochem.2012.04.013	journal	August 2012
Optics upgrades at the APS beamline 20-BM Heald, Steve M. Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 649, Issue 1 https://doi.org/10.1016/j.nima.2010.11.070	journal	September 2011
XAFS and micro-XAFS at the PNC-CAT beamlines Heald, S. M.; Brewe, D. L.; Stern, E. A. Journal of Synchrotron Radiation, Vol. 6, Issue 3 https://doi.org/10.1107/S090904959801677X	journal	May 1999
ATHENA , ARTEMIS , HEPHAESTUS : data analysis for X-ray absorption spectroscopy using IFEFFIT Ravel, B.; Newville, M. Journal of Synchrotron Radiation, Vol. 12, Issue 4 https://doi.org/10.1107/S0909049505012719	journal	June 2005
IFEFFIT : interactive XAFS analysis and FEFF fitting Newville, Matthew Journal of Synchrotron Radiation, Vol. 8, Issue 2 https://doi.org/10.1107/S0909049500016964	journal	March 2001
Monovalent Cations in Structures of the Meta-Autunite Group Locock, A. J.; Burns, P. C.; Duke, M. J. M. The Canadian Mineralogist, Vol. 42, Issue 4 https://doi.org/10.2113/gscanmin.42.4.973	journal	August 2004
Divalent Transition Metals and Magnesium in Structures that Contain the Autunite-Type Sheet Locock, A. J.; Burns, P. C.; Flynn, T. M. The Canadian Mineralogist, Vol. 42, Issue 6 https://doi.org/10.2113/gscanmin.42.6.1699	journal	December 2004
Hydrogen uranyl phosphate tetrahydrate, a hydrogen ion solid electrolyte Morosin, B. Acta Crystallographica Section B Structural Crystallography and Crystal Chemistry, Vol. 34, Issue 12 https://doi.org/10.1107/S0567740878011991	journal	December 1978
Analysis of uranyl-bearing phases by EXAFS spectroscopy: Interferences, multiple scattering, accuracy of structural parameters, and spectral differences Catalano, Jeffrey G.; Brown, Gordon E. American Mineralogist, Vol. 89, Issue 7 https://doi.org/10.2138/am-2004-0711	journal	July 2004
Sequential extraction procedure for the speciation of particulate trace metals Tessier, A.; Campbell, P. G. C.; Bisson, M. Analytical Chemistry, Vol. 51, Issue 7 https://doi.org/10.1021/ac50043a017	journal	June 1979
Cryogenic Laser Induced Fluorescence Characterization of U(VI) in Hanford Vadose Zone Pore Waters Wang, Zheming; Zachara, John M.; Yantasee, Wassana Environmental Science & Technology, Vol. 38, Issue 21 https://doi.org/10.1021/es049512u	journal	November 2004
Fluorescence spectroscopy of U(VI)-silicates and U(VI)-contaminated Hanford sediment Wang, Zheming; Zachara, John M.; Gassman, Paul L. Geochimica et Cosmochimica Acta, Vol. 69, Issue 6 https://doi.org/10.1016/j.gca.2004.08.028	journal	March 2005
Impact of Uranyl−Calcium−Carbonato Complexes on Uranium(VI) Adsorption to Synthetic and Natural Sediments Stewart, Brandy D.; Mayes, Melanie A.; Fendorf, Scott Environmental Science & Technology, Vol. 44, Issue 3 https://doi.org/10.1021/es902194x	journal	February 2010
Effect of phosphate on U(VI) sorption to montmorillonite: Ternary complexation and precipitation barriers Troyer, Lyndsay D.; Maillot, Fabien; Wang, Zheming Geochimica et Cosmochimica Acta, Vol. 175 https://doi.org/10.1016/j.gca.2015.11.029	journal	February 2016
Microscopic reactive diffusion of uranium in the contaminated sediments at Hanford, United States: MICROSCOPIC REACTIVE DIFFUSION Liu, Chongxuan; Zachara, John M.; Yantasee, Wassana Water Resources Research, Vol. 42, Issue 12 https://doi.org/10.1029/2006WR005031	journal	December 2006
Study of Sorption-Retarded U(VI) Diffusion in Hanford Silt/Clay Material Bai, Jing; Liu, Chongxuan; Ball, William P. Environmental Science & Technology, Vol. 43, Issue 20 https://doi.org/10.1021/es901306c	journal	October 2009
Kinetics of Uranium(VI) Desorption from Contaminated Sediments: Effect of Geochemical Conditions and Model Evaluation Liu, Chongxuan; Shi, Zhenqing; Zachara, John M. Environmental Science & Technology, Vol. 43, Issue 17 https://doi.org/10.1021/es900666m	journal	September 2009
A cryogenic fluorescence spectroscopic study of uranyl carbonate, phosphate and oxyhydroxide minerals Wang, Zheming; Zachara, John M.; Liu, Chongxuan Radiochimica Acta, Vol. 96, Issue 9-11 https://doi.org/10.1524/ract.2008.1541	journal	November 2008
Determining individual mineral contributions to U(VI) adsorption in a contaminated aquifer sediment: A fluorescence spectroscopy study Wang, Zheming; Zachara, John M.; Boily, Jean-François Geochimica et Cosmochimica Acta, Vol. 75, Issue 10 https://doi.org/10.1016/j.gca.2011.03.008	journal	May 2011

Cited By (1)

Transport and transformation of uranium and heavy metals from uranium tailings under simulated rain at different pH Liu, Bo; Sun, Hongjuan; Peng, Tongjiang Environmental Chemistry Letters, Vol. 18, Issue 2 https://doi.org/10.1007/s10311-019-00951-4	journal	November 2019

Similar Records

Phosphate-Induced Immobilization of Uranium in Hanford Sediments

Journal Article · Tue Dec 20 00:00:00 EST 2016 · Environmental Science and Technology · OSTI ID:1346213

Pan, Zezhen; Giammar, Daniel E.; Mehta, Vrajesh; +3 more

Transport of U(VI) through sediments amended with phosphate to induce in situ uranium immobilization

Journal Article · Sun Feb 01 00:00:00 EST 2015 · Water Research · OSTI ID:1346213

Mehta, Vrajesh S.; Maillot, Fabien; Wang, Zheming; +2 more

Final Report: Dominant Mechanisms of Uranium-Phosphate Reactions in Subsurface Sediments

Technical Report · Tue Mar 08 00:00:00 EST 2016 · OSTI ID:1346213

Catalano, Jeffrey G.; Giammar, Daniel E.; Wang, Zheming

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
geological materials
Uranium
adsorption
immobilization
phosphates

Title: Phosphate-Induced Immobilization of Uranium in Hanford Sediments

Citation Formats

References (39)

Cited By (1)

Similar Records

Related Subjects