Effect of fulvic acid surface coatings on plutonium sorption and desorption kinetics on goethite

Tinnacher, Ruth M.; Begg, James D.; Mason, Harris; Ranville, James; Powell, Brian A.; Wong, Jennifer C.; Kersting, Annie B.; Zavarin, Mavrik

doi:10.1021/es505120s

Title: Effect of fulvic acid surface coatings on plutonium sorption and desorption kinetics on goethite

Journal Article · Wed Jan 21 00:00:00 EST 2015 · Environmental Science and Technology

DOI:https://doi.org/10.1021/es505120s· OSTI ID:1266683

Tinnacher, Ruth M. ^[1]; Begg, James D. ^[2]; Mason, Harris ^[2]; Ranville, James ^[3]; Powell, Brian A. ^[4]; Wong, Jennifer C. ^[4]; Kersting, Annie B. ^[2]; Zavarin, Mavrik ^[2]

Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Colorado School of Mines, Golden, CO (United States)
Clemson Univ., Clemson, SC (United States)

The rates and extent of plutonium (Pu) sorption and desorption onto mineral surfaces are important parameters for predicting Pu mobility in subsurface environments. The presence of natural organic matter, such as fulvic acid (FA), may influence these parameters. We investigated the effects of FA on Pu(IV) sorption/desorption onto goethite in two scenarios: when FA was (1) initially present in solution or (2) found as organic coatings on the mineral surface. A low pH was used to maximize FA coatings on goethite. Experiments were combined with kinetic modeling and speciation calculations to interpret variations in Pu sorption rates in the presence of FA. Our results indicate that FA can change the rates and extent of Pu sorption onto goethite at pH 4. Differences in the kinetics of Pu sorption were observed as a function of the concentration and initial form of FA. The fraction of desorbed Pu decreased in the presence of FA, indicating that organic matter can stabilize sorbed Pu on goethite. These results suggest that ternary Pu–FA–mineral complexes could enhance colloid-facilitated Pu transport. In conclusion, more representative natural conditions need to be investigated to quantify the relevance of these findings.

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Research Organization:: Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)

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

Grant/Contract Number:: AC52-07NA27344

OSTI ID:: 1266683

Report Number(s):: LLNL-JRNL-663069

Journal Information:: Environmental Science and Technology, Vol. 49, Issue 5; ISSN 0013-936X

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 31 works

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References (46)

Sorption of dissolved organic carbon by hydrous aluminum and iron oxides occurring at the confluence of Deer Creek with the Snake River, Summit County, Colorado McKnight, Diane M.; Bencala, Kenneth E.; Zellweger, Gary W. Environmental Science & Technology, Vol. 26, Issue 7 https://doi.org/10.1021/es00031a017	journal	July 1992
Redox speciation of plutonium in natural waters Choppin, G. R. Journal of Radioanalytical and Nuclear Chemistry Articles, Vol. 147, Issue 1 https://doi.org/10.1007/BF02039572	journal	January 1991
Influence of humic acid on plutonium sorption to gibbsite: Determination of Pu-humic acid complexation constants and ternary sorption studies Zimmerman, Trevor; Zavarin, Mavrik; Powell, Brian A. Radiochimica Acta, Vol. 102, Issue 7 https://doi.org/10.1515/ract-2014-2163	journal	January 2014
Plutonium in groundwater at the 100K-Area of the U.S. DOE Hanford Site Dai, Minhan; Buesseler, Ken O.; Pike, Steven M. Journal of Contaminant Hydrology, Vol. 76, Issue 3-4 https://doi.org/10.1016/j.jconhyd.2004.08.004	journal	February 2005
Colloid properties in granitic groundwater systems. I: Sampling and characterisation Degueldre, C.; Pfeiffer, H. -R.; Alexander, W. Applied Geochemistry, Vol. 11, Issue 5 https://doi.org/10.1016/S0883-2927(96)00036-4	journal	September 1996
Actinide Carbonte Complexes and Their Importance in Actinide Environmental Chemistry Clark, David L.; Hobart, David E.; Neu, Mary P. Chemical Reviews, Vol. 95, Issue 1 https://doi.org/10.1021/cr00033a002	journal	January 1995
Kinetics of neptunium(V) sorption and desorption on goethite: An experimental and modeling study Tinnacher, Ruth M.; Zavarin, Mavrik; Powell, Brian A. Geochimica et Cosmochimica Acta, Vol. 75, Issue 21 https://doi.org/10.1016/j.gca.2011.08.014	journal	November 2011
Eleven-Year Field Study of Pu Migration from Pu III, IV, and VI Sources Kaplan, Daniel I.; Demirkanli, Deniz I.; Gumapas, Leo Environmental Science & Technology, Vol. 40, Issue 2 https://doi.org/10.1021/es050073o	journal	January 2006
Plutonium Partitioning to Colloidal and Particulate Matter in an Acidic, Sandy Sediment: Implications for Remediation Alternatives and Plutonium Migration Loyland Asbury, S. M.; Lamont, S. P.; Clark, S. B. Environmental Science & Technology, Vol. 35, Issue 11 https://doi.org/10.1021/es001697r	journal	June 2001
Pu(V)O ₂ ⁺ Adsorption and Reduction by Synthetic Magnetite (Fe ₃ O ₄ ) Powell, Brian A.; Fjeld, Robert A.; Kaplan, Daniel I. Environmental Science & Technology, Vol. 38, Issue 22 https://doi.org/10.1021/es049386u	journal	November 2004
A New Method to Radiolabel Natural Organic Matter by Chemical Reduction with Tritiated Sodium Borohydride Tinnacher, Ruth M.; Honeyman, Bruce D. Environmental Science & Technology, Vol. 41, Issue 19 https://doi.org/10.1021/es070563b	journal	October 2007
Source-Dependent and Source-Independent Controls on Plutonium Oxidation State and Colloid Associations in Groundwater Buesseler, Ken O.; Kaplan, Daniel I.; Dai, Minhan Environmental Science & Technology, Vol. 43, Issue 5 https://doi.org/10.1021/es8028318	journal	January 2009
Role of colloids and humic substances in the transport of radio-elements through the geosphere Moulin, V.; Ouzounian, G. Applied Geochemistry, Vol. 7 https://doi.org/10.1016/S0883-2927(09)80074-7	journal	January 1992
Plutonium(III) complexation by humic substances studied by X-ray absorption fine structure spectroscopy Schmeide, Katja; Reich, Tobias; Sachs, Susanne Inorganica Chimica Acta, Vol. 359, Issue 1 https://doi.org/10.1016/j.ica.2005.10.037	journal	January 2006
Redox speciation of plutonium Choppin, G. R.; Bond, A. H.; Hromadka, P. M. Journal of Radioanalytical and Nuclear Chemistry, Vol. 219, Issue 2 https://doi.org/10.1007/BF02038501	journal	May 1997
Influence of Natural Organic Matter on the Adsorption of Metal Ions onto Clay Minerals Schmitt, D.; Taylor, H. E.; Aiken, G. R. Environmental Science & Technology, Vol. 36, Issue 13 https://doi.org/10.1021/es010271p	journal	July 2002
Determination of Stability Constants of U(VI)−Fe(III)−Citrate Complexes Kantar, Cetin; Gillow, Jeff B.; Harper-Arabie, Ruth Environmental Science & Technology, Vol. 39, Issue 7 https://doi.org/10.1021/es048852c	journal	April 2005
Two-Dimensional NMR Studies of Size Fractionated Suwannee River Fulvic and Humic Acid Reference Haiber, S.; Herzog, H.; Burba, P. Environmental Science & Technology, Vol. 35, Issue 21 https://doi.org/10.1021/es010033u	journal	November 2001
Complexation of Pu(IV) with the Natural Siderophore Desferrioxamine B and the Redox Properties of Pu(IV)(siderophore) Complexes Boukhalfa, Hakim; Reilly, Sean D.; Neu, Mary P. Inorganic Chemistry, Vol. 46, Issue 3 https://doi.org/10.1021/ic061544q	journal	February 2007
Environmental impact of the nuclear fuel cycle: Fate of actinides Ewing, Rodney C.; Runde, Wolfgang; Albrecht-Schmitt, Thomas E. MRS Bulletin, Vol. 35, Issue 11 https://doi.org/10.1557/mrs2010.712	journal	November 2010
Influence of Sources on Plutonium Mobility and Oxidation State Transformations in Vadose Zone Sediments Kaplan, Daniel I.; Powell, Brian A.; Duff, Martine C. Environmental Science & Technology, Vol. 41, Issue 21 https://doi.org/10.1021/es0706302	journal	November 2007
Speciation and interactions of plutonium with humic substances and kaolinite in aquifer systems Banik, N. L.; Buda, R. A.; Bürger, S. Journal of Alloys and Compounds, Vol. 444-445 https://doi.org/10.1016/j.jallcom.2006.12.048	journal	October 2007
Solubility and hydrolysis of tetravalent actinides Neck, Volker; Kim, J. I. Radiochimica Acta, Vol. 89, Issue 1 https://doi.org/10.1524/ract.2001.89.1.001	journal	January 2001
The adsorption of plutonium IV and V on goethite Sanchez, Arthur L.; Murray, James W.; Sibley, Thomas H. Geochimica et Cosmochimica Acta, Vol. 49, Issue 11 https://doi.org/10.1016/0016-7037(85)90230-3	journal	November 1985
Pu(V) and Pu(IV) Sorption to Montmorillonite Begg, James D.; Zavarin, Mavrik; Zhao, Pihong Environmental Science & Technology, Vol. 47, Issue 10 https://doi.org/10.1021/es305257s	journal	May 2013
The role of sorbed humic substances on the distribution of organic and inorganic contaminants in groundwater Murphy, E. M.; Zachara, J. M. Geoderma, Vol. 67, Issue 1-2 https://doi.org/10.1016/0016-7061(94)00055-F	journal	June 1995
Organic Nature of Colloidal Actinides Transported in Surface Water Environments Santschi, Peter H.; Roberts, Kimberly A.; Guo, Laodong Environmental Science & Technology, Vol. 36, Issue 17 https://doi.org/10.1021/es0112588	journal	September 2002
Redox interactions of Pu(V) in solutions containing different humic substances Blinova, Oxana; Novikov, Alexandr; Perminova, Irina Journal of Alloys and Compounds, Vol. 444-445 https://doi.org/10.1016/j.jallcom.2007.02.117	journal	October 2007
Pu(V)O ₂ ⁺ Adsorption and Reduction by Synthetic Hematite and Goethite Powell, Brian A.; Fjeld, Robert A.; Kaplan, Daniel I. Environmental Science & Technology, Vol. 39, Issue 7 https://doi.org/10.1021/es0487168	journal	April 2005
Plutonium Transport in the Environment Kersting, Annie B. Inorganic Chemistry, Vol. 52, Issue 7 https://doi.org/10.1021/ic3018908	journal	June 2012
Effect of ionic strength on complexation of Pu(IV) with humic acid Szabo, Gyula; Guczi, J.; Reiller, Pascal E. Radiochimica Acta, Vol. 98, Issue 1 https://doi.org/10.1524/ract.2010.1683	journal	January 2010
The redox chemistry of Pu(V)O2+ interaction with common mineral surfaces in dilute solutions and seawater Keeney-kennicutt, Wendy L.; Morse, John W. Geochimica et Cosmochimica Acta, Vol. 49, Issue 12 https://doi.org/10.1016/0016-7037(85)90127-9	journal	December 1985
Sources and Migration of Plutonium in Groundwater at the Savannah River Site Dai, Minhan; Kelley, James M.; Buesseler, Ken O. Environmental Science & Technology, Vol. 36, Issue 17 https://doi.org/10.1021/es020025t	journal	September 2002
Colloidal α-Al ₂ O _3, Europium(III) and Humic Substances Interactions: A Macroscopic and Spectroscopic Study Janot, Noémie; Benedetti, Marc F.; Reiller, Pascal E. Environmental Science & Technology, Vol. 45, Issue 8 https://doi.org/10.1021/es102592a	journal	April 2011
Actinide Sorption in Rainier Mesa Tunnel Waters from the Nevada Test Site Zhao, P.; Zavarin, M.; Leif, R. https://doi.org/10.2172/926020	report	December 2007
Plutonium Immobilization and Remobilization by Soil Mineral and Organic Matter in the Far-Field of the Savannah River Site, U.S. Xu, Chen; Athon, Matthew; Ho, Yi-Fang Environmental Science & Technology, Vol. 48, Issue 6 https://doi.org/10.1021/es404951y	journal	March 2014
Characterization of organic-rich colloids from surface and ground waters at the actinide-contaminated Rocky Flats Environmental Technology Site (RFETS), Colorado, USA Roberts, Kimberly A.; Santschi, Peter H.; Leppard, Gary G. Colloids and Surfaces A: Physicochemical and Engineering Aspects, Vol. 244, Issue 1-3 https://doi.org/10.1016/j.colsurfa.2004.06.009	journal	September 2004
Colloid Transport of Plutonium in the Far-Field of the Mayak Production Association, Russia Novikov, A. P.; Kalmykov, S. N.; Utsunomiya, S. Science, Vol. 314, Issue 5799 https://doi.org/10.1126/science.1131307	journal	October 2006
Mobilization of actinides by dissolved organic compounds at the Nevada Test Site Zhao, Pihong; Zavarin, Mavrik; Leif, Roald N. Applied Geochemistry, Vol. 26, Issue 3 https://doi.org/10.1016/j.apgeochem.2010.12.004	journal	March 2011
Migration of plutonium in ground water at the Nevada Test Site Kersting, A. B.; Efurd, D. W.; Finnegan, D. L. Nature, Vol. 397, Issue 6714 https://doi.org/10.1038/16231	journal	January 1999
Influence of Oxidation States on Plutonium Mobility during Long-Term Transport through an Unsaturated Subsurface Environment Kaplan, Daniel I.; Powell, Brian A.; Demirkanli, Deniz I. Environmental Science & Technology, Vol. 38, Issue 19 https://doi.org/10.1021/es049406s	journal	October 2004
Actinide Colloid Generation in Groundwater Kim, J. I. Radiochimica Acta, Vol. 52-53, Issue 1 https://doi.org/10.1524/ract.1991.5253.1.71	journal	January 1991
Pu(V) reduction and enhancement of particle-water partitioning by exopolymeric substances Roberts, Kimberly A.; Santschi, Peter H.; Honeyman, Bruce D. Radiochimica Acta, Vol. 96, Issue 9-11 https://doi.org/10.1524/ract.2008.1560	journal	November 2008
Studies of the ternary systems humic substances – kaolinite – Pu(III) and Pu(IV) Buda, R.; Banik, N. L.; Kratz, Jens Volker Radiochimica Acta, Vol. 96, Issue 9-11 https://doi.org/10.1524/ract.2008.1550	journal	January 2008
Comparison of Chemical Extractions and Laser Photoacoustic Spectroscopy for the Determination of Plutonium Species in Near-Neutral Carbonate Solutions Neu, Mary P.; Hoffman, Darleane C.; Roberts, Kevin E. Radiochimica Acta, Vol. 66-67, Issue s1 https://doi.org/10.1524/ract.1994.6667.s1.251	journal	December 1994
The redox behaviour of plutonium in humic rich groundwater Marquardt, Christian M.; Seibert, A.; Artinger, Robert Radiochimica Acta, Vol. 92, Issue 9-11 https://doi.org/10.1524/ract.92.9.617.55007	journal	January 2004

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Title: Effect of fulvic acid surface coatings on plutonium sorption and desorption kinetics on goethite

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