Effect of Natural Organic Matter on Plutonium Sorption to Goethite
Abstract
For this research, the effect of citric acid (CA), desferrioxamine B (DFOB), fulvic acid (FA), and humic acid (HA) on plutonium (Pu) sorption to goethite was studied as a function of organic carbon concentration and pH using batch sorption experiments at 5 mgC·L–1 and 50 mgC·L–1 natural organic matter (NOM), 10–9–10–10 M 238Pu, and 0.1 g·L–1 goethite concentrations, at pH 3, 5, 7, and 9. Low sorption of ligands coupled with strong Pu complexation decreased Pu sorption at pH 5 and 7, relative to a ligand-free system. Conversely, CA, FA, and HA increased Pu sorption to goethite at pH 3, suggesting ternary complex formation or, in the case of humic acid, incorporation into HA aggregates. Mechanisms for ternary complex formation were characterized by Fourier transform infrared spectroscopy in the absence of Pu. CA and FA demonstrated clear surface interactions at pH 3, HA appeared unchanged suggesting HA aggregates had formed, and no DFOB interactions were observed. Plutonium sorption decreased in the presence of DFOB (relative to a ligand free system) at all pH values examined. Thus, DFOB does not appear to facilitate formation of ternary Pu-DFOB-goethite complexes. At pH 9, Pu sorption in the presence of all NOM increased relativemore »
- Authors:
-
- Clemson Univ., SC (United States). Department of Environmental Engineering and Earth Sciences
- Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States). Glenn T. Seaborg Institute, Physical and Life Sciences Directorate
- Clemson Univ., SC (United States). Department of Environmental Engineering and Earth Sciences
- Publication Date:
- Research Org.:
- Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Biological and Environmental Research (BER)
- OSTI Identifier:
- 1409924
- Report Number(s):
- LLNL-JRNL-734915
Journal ID: ISSN 0013-936X
- Grant/Contract Number:
- AC52-07NA27344
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Environmental Science and Technology
- Additional Journal Information:
- Journal Volume: 51; Journal Issue: 1; Journal ID: ISSN 0013-936X
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 54 ENVIRONMENTAL SCIENCES; 58 GEOSCIENCES; 38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY
Citation Formats
Conroy, Nathan A., Zavarin, Mavrik, Kersting, Annie B., and Powell, Brian A. Effect of Natural Organic Matter on Plutonium Sorption to Goethite. United States: N. p., 2016.
Web. doi:10.1021/acs.est.6b03587.
Conroy, Nathan A., Zavarin, Mavrik, Kersting, Annie B., & Powell, Brian A. Effect of Natural Organic Matter on Plutonium Sorption to Goethite. United States. https://doi.org/10.1021/acs.est.6b03587
Conroy, Nathan A., Zavarin, Mavrik, Kersting, Annie B., and Powell, Brian A. Mon .
"Effect of Natural Organic Matter on Plutonium Sorption to Goethite". United States. https://doi.org/10.1021/acs.est.6b03587. https://www.osti.gov/servlets/purl/1409924.
@article{osti_1409924,
title = {Effect of Natural Organic Matter on Plutonium Sorption to Goethite},
author = {Conroy, Nathan A. and Zavarin, Mavrik and Kersting, Annie B. and Powell, Brian A.},
abstractNote = {For this research, the effect of citric acid (CA), desferrioxamine B (DFOB), fulvic acid (FA), and humic acid (HA) on plutonium (Pu) sorption to goethite was studied as a function of organic carbon concentration and pH using batch sorption experiments at 5 mgC·L–1 and 50 mgC·L–1 natural organic matter (NOM), 10–9–10–10 M 238Pu, and 0.1 g·L–1 goethite concentrations, at pH 3, 5, 7, and 9. Low sorption of ligands coupled with strong Pu complexation decreased Pu sorption at pH 5 and 7, relative to a ligand-free system. Conversely, CA, FA, and HA increased Pu sorption to goethite at pH 3, suggesting ternary complex formation or, in the case of humic acid, incorporation into HA aggregates. Mechanisms for ternary complex formation were characterized by Fourier transform infrared spectroscopy in the absence of Pu. CA and FA demonstrated clear surface interactions at pH 3, HA appeared unchanged suggesting HA aggregates had formed, and no DFOB interactions were observed. Plutonium sorption decreased in the presence of DFOB (relative to a ligand free system) at all pH values examined. Thus, DFOB does not appear to facilitate formation of ternary Pu-DFOB-goethite complexes. At pH 9, Pu sorption in the presence of all NOM increased relative to pH 5 and 7; speciation models attributed this to Pu(IV) hydrolysis competing with ligand complexation, increasing sorption. In conclusion, the results indicate that in simple Pu-NOM-goethite ternary batch systems, NOM will decrease Pu sorption to goethite at all but particularly low pH conditions.},
doi = {10.1021/acs.est.6b03587},
journal = {Environmental Science and Technology},
number = 1,
volume = 51,
place = {United States},
year = {Mon Nov 21 00:00:00 EST 2016},
month = {Mon Nov 21 00:00:00 EST 2016}
}
Web of Science
Works referenced in this record:
Plutonium Transport in the Environment
journal, June 2012
- Kersting, Annie B.
- Inorganic Chemistry, Vol. 52, Issue 7
Organic Nature of Colloidal Actinides Transported in Surface Water Environments
journal, September 2002
- Santschi, Peter H.; Roberts, Kimberly A.; Guo, Laodong
- Environmental Science & Technology, Vol. 36, Issue 17
Migration of plutonium in ground water at the Nevada Test Site
journal, January 1999
- Kersting, A. B.; Efurd, D. W.; Finnegan, D. L.
- Nature, Vol. 397, Issue 6714
The adsorption of plutonium IV and V on goethite
journal, November 1985
- Sanchez, Arthur L.; Murray, James W.; Sibley, Thomas H.
- Geochimica et Cosmochimica Acta, Vol. 49, Issue 11
Plutonium sorption onto hematite colloids at femto- and nanomolar concentrations
journal, March 2011
- Romanchuk, Anna Yu.; Kalmykov, Stepan N.; Aliev, Ramiz A.
- Radiochimica Acta, Vol. 99, Issue 3
The redox chemistry of Pu(V)O2+ interaction with common mineral surfaces in dilute solutions and seawater
journal, December 1985
- Keeney-kennicutt, Wendy L.; Morse, John W.
- Geochimica et Cosmochimica Acta, Vol. 49, Issue 12
Pu(V)O 2 + Adsorption and Reduction by Synthetic Magnetite (Fe 3 O 4 )
journal, November 2004
- Powell, Brian A.; Fjeld, Robert A.; Kaplan, Daniel I.
- Environmental Science & Technology, Vol. 38, Issue 22
Oxidation State and Local Structure of Plutonium Reacted with Magnetite, Mackinawite, and Chukanovite
journal, September 2011
- Kirsch, Regina; Fellhauer, David; Altmaier, Marcus
- Environmental Science & Technology, Vol. 45, Issue 17
Colloid Transport of Plutonium in the Far-Field of the Mayak Production Association, Russia
journal, October 2006
- Novikov, A. P.; Kalmykov, S. N.; Utsunomiya, S.
- Science, Vol. 314, Issue 5799
Mobilization of actinides by dissolved organic compounds at the Nevada Test Site
journal, March 2011
- Zhao, Pihong; Zavarin, Mavrik; Leif, Roald N.
- Applied Geochemistry, Vol. 26, Issue 3
The effects of humic substances on the transport of radionuclides: Recent improvements in the prediction of behaviour and the understanding of mechanisms
journal, February 2012
- Bryan, Nick D.; Abrahamsen, Liam; Evans, Nick
- Applied Geochemistry, Vol. 27, Issue 2
Adsorption and desorption of natural organic matter on iron oxide: mechanisms and models
journal, January 1994
- Gu, Baohua.; Schmitt, Juergen.; Chen, Zhihong.
- Environmental Science & Technology, Vol. 28, Issue 1
Sorption and Fractionation of a Peat Derived Humic Acid by Kaolinite, Montmorillonite, and Goethite
journal, February 2009
- Ghosh, S.; Wang, Zhen-Yu; Kang, S.
- Pedosphere, Vol. 19, Issue 1
Humic Acid Fractionation upon Sequential Adsorption onto Goethite
journal, February 2008
- Kang, Seunghun; Xing, Baoshan
- Langmuir, Vol. 24, Issue 6
Adsorption of (poly)maleic acid and an aquatic fulvic acid by geothite
journal, December 1997
- Wang, Lili; Chin, Yu-Ping; Traina, Samuel J.
- Geochimica et Cosmochimica Acta, Vol. 61, Issue 24
Adsorption of humic acids onto goethite: Effects of molar mass, pH and ionic strength
journal, October 2007
- Weng, Liping; Van Riemsdijk, Willem H.; Hiemstra, Tjisse
- Journal of Colloid and Interface Science, Vol. 314, Issue 1
Effect of Fulvic Acid Surface Coatings on Plutonium Sorption and Desorption Kinetics on Goethite
journal, February 2015
- Tinnacher, Ruth M.; Begg, James D.; Mason, Harris
- Environmental Science & Technology, Vol. 49, Issue 5
Studies of the ternary systems humic substances – kaolinite – Pu(III) and Pu(IV)
journal, January 2008
- Buda, R.; Banik, N. L.; Kratz, Jens Volker
- Radiochimica Acta, Vol. 96, Issue 9-11
Influence of humic acid on plutonium sorption to gibbsite: Determination of Pu-humic acid complexation constants and ternary sorption studies
journal, January 2014
- Zimmerman, Trevor; Zavarin, Mavrik; Powell, Brian A.
- Radiochimica Acta, Vol. 102, Issue 7
The influence of natural organic matter on radionuclide mobility under conditions relevant to cementitious disposal of radioactive wastes: A review of direct evidence
journal, June 2013
- Stockdale, Anthony; Bryan, Nick D.
- Earth-Science Reviews, Vol. 121
A New Method to Radiolabel Natural Organic Matter by Chemical Reduction with Tritiated Sodium Borohydride
journal, October 2007
- Tinnacher, Ruth M.; Honeyman, Bruce D.
- Environmental Science & Technology, Vol. 41, Issue 19
Plutonium Oxidation and Subsequent Reduction by Mn(IV) Minerals in Yucca Mountain Tuff
journal, May 2006
- Powell, Brian A.; Duff, Martine C.; Kaplan, Daniel I.
- Environmental Science & Technology, Vol. 40, Issue 11
A Novel Method for Tracer Concentration Plutonium(V) Solution Preparation
journal, March 2016
- Conroy, Nathan A.; Wylie, E. Miller; Powell, Brian A.
- Analytical Chemistry, Vol. 88, Issue 8
Plutonium(III,IV,VI) speciation in Gorleben groundwater using XAFS
journal, January 2009
- Dardenne, Kathy; Seibert, Alice; Denecke, Melissa A.
- Radiochimica Acta, Vol. 97, Issue 2
Actinide speciation in the environment
journal, January 2003
- Choppin, Gregory R.
- Radiochimica Acta, Vol. 91, Issue 11
Reduction of Pu(V) by humic acid
journal, January 2000
- André, C.; Choppin, Gregory R.
- Radiochimica Acta, Vol. 88, Issue 9-11
The redox behaviour of plutonium in humic rich groundwater
journal, January 2004
- Marquardt, Christian M.; Seibert, A.; Artinger, Robert
- Radiochimica Acta, Vol. 92, Issue 9-11
Influence of Oxidation States on Plutonium Mobility during Long-Term Transport through an Unsaturated Subsurface Environment
journal, October 2004
- Kaplan, Daniel I.; Powell, Brian A.; Demirkanli, Deniz I.
- Environmental Science & Technology, Vol. 38, Issue 19
Limits for qualitative detection and quantitative determination. Application to radiochemistry
journal, March 1968
- Currie, Lloyd A.
- Analytical Chemistry, Vol. 40, Issue 3
Surface effects in photochemistry: an in situ cylindrical internal reflection-Fourier transform infrared investigation of the effect of ring substituents on chemisorption onto titania ceramic membranes
journal, February 1992
- Tunesi, Simonetta; Anderson, Marc A.
- Langmuir, Vol. 8, Issue 2
Characterization of benzoic and phenolic complexes at the goethite/aqueous solution interface using cylindrical internal reflection Fourier transform infrared spectroscopy. Part 1. Methodology
journal, May 1990
- Tejedor-Tejedor, M. Isabel; Yost, Eric C.; Anderson, Marc A.
- Langmuir, Vol. 6, Issue 5
In situ CIR-FTIR characterization of salicylate complexes at the goethite/aqueous solution interface
journal, June 1990
- Yost, Eric C.; Tejedor-Tejedor, M. Isabel; Anderson, Marc A.
- Environmental Science & Technology, Vol. 24, Issue 6
Complexation of Pu(IV) with the Natural Siderophore Desferrioxamine B and the Redox Properties of Pu(IV)(siderophore) Complexes
journal, February 2007
- Boukhalfa, Hakim; Reilly, Sean D.; Neu, Mary P.
- Inorganic Chemistry, Vol. 46, Issue 3
Infrared spectrum and ab initio calculations of matrix isolated methanesulfonic acid species and its 1:1 water complex
journal, June 2005
- Givan, A.; Loewenschuss, A.; Nielsen, C. J.
- Journal of Molecular Structure, Vol. 748, Issue 1-3
Sorption of U(VI) on goethite: Effects of pH, ionic strength, phosphate, carbonate and fulvic acid
journal, June 2009
- Guo, Zhijun; Li, Yan; Wu, Wangsuo
- Applied Radiation and Isotopes, Vol. 67, Issue 6
Complexes of fulvic acid on the surface of hematite, goethite, and akaganeite: FTIR observation
journal, April 2006
- Fu, Hongbo; Quan, Xie
- Chemosphere, Vol. 63, Issue 3
Characterization of hematite and its interaction with humic material using flow field-flow fractionation
journal, August 1998
- Petteys, Mark P.; Schimpf, Martin E.
- Journal of Chromatography A, Vol. 816, Issue 2
Extraction of Plutonium by Chelating Hydroxypyridinone and Catecholamide Resins∗
journal, September 1999
- Zhao, Pihong; Romanovski, Vadim V.; Whisenhunt, Donald W.
- Solvent Extraction and Ion Exchange, Vol. 17, Issue 5
Thermodynamic Modeling of the Adsorption of Radionuclides on Selected Minerals. I: Cations
journal, October 2001
- Wang, Peiming; Anderko, Andrzej; Turner, David R.
- Industrial & Engineering Chemistry Research, Vol. 40, Issue 20
Retention behaviour of humic substances onto mineral surfaces and consequences upon thorium (IV) mobility: case of iron oxides
journal, December 2002
- Reiller, Pascal; Moulin, Valérie; Casanova, Florence
- Applied Geochemistry, Vol. 17, Issue 12
Interaction of humic and fulvic acids with Th(IV)
journal, January 1980
- Nash, Kenneth L.; Choppin, Gregory R.
- Journal of Inorganic and Nuclear Chemistry, Vol. 42, Issue 7