Hostname: page-component-848d4c4894-5nwft Total loading time: 0 Render date: 2024-06-07T22:54:57.848Z Has data issue: false hasContentIssue false
  • English
  • Français

Interactions of Radioactive and Stable Cesium with Hydroxy-Interlayered Vermiculite Grains in Soils of the Savannah River Site, South Carolina, USA

Published online by Cambridge University Press:  01 January 2024

Momoko Goto ,
Robert Rosson ,
W. Crawford Elliott ,
J. M. Wampler ,
Steven Serkiz  and
Bernd Kahn
Momoko Goto
Affiliation:
Woodruff School of Mechanical Engineering, Georgia Institute of Technology, 30332-0405, Atlanta, GA, USA Current name and affiliation: Momoko Tajiri, Department of Chemistry, Michigan Technological University, 49931, Houghton, MI, USA
Robert Rosson
Affiliation:
Environmental Radiation Center, EOSL, GTRI, Georgia Institute of Technology, 30332-0826, Atlanta, GA, USA
W. Crawford Elliott
Affiliation:
Department of Geosciences, Georgia State University, 30302-4105, Atlanta, GA, USA
J. M. Wampler*
Affiliation:
Department of Geosciences, Georgia State University, 30302-4105, Atlanta, GA, USA School of Earth and Atmospheric Sciences, Georgia Institute of Technology, 30332-0340, Atlanta, GA, USA
Steven Serkiz
Affiliation:
Savannah River National Laboratory, 29808, Aiken, SC, USA Environmental Engineering and Earth Sciences, Clemson University, 29634, Clemson, SC, USA
Bernd Kahn
Affiliation:
Woodruff School of Mechanical Engineering, Georgia Institute of Technology, 30332-0405, Atlanta, GA, USA Environmental Radiation Center, EOSL, GTRI, Georgia Institute of Technology, 30332-0826, Atlanta, GA, USA
*
*E-mail address of corresponding author: wampler@eas.gatech.edu
Get access Rights & Permissions [Opens in a new window]

Abstract

Sorption and fixation of Cs by the upland soils of the US Department of Energy’s Savannah River Site (SRS) have been attributed to micaceous grains consisting mostly of hydroxy-interlayered vermiculite (HIV). Results of experiments to characterize SRS soil samples, to examine aspects of their radiocesium sorption, and to determine how much of their natural Cs is accessible for chemical extraction and isotope dilution are presented in support of mechanistic hypotheses to explain Cs sorption and fixation in HIV grains. The HIV is responsible for most of the soil cation exchange capacity, and concentrations of naturally occurring Cs, Rb, and K in soil samples are closely related to the concentration of HIV. Experiments with 137Cs to examine (1) sorption kinetics, (2) blocking of exchange sites with silver thiourea, and (3) susceptibility of sorbed 137Cs to chemical extraction, support the idea that added Cs is sorbed at different kinds of cation exchange sites in HIV grains. Sites highly selective for Cs but relatively few in number are inferred to exist in interlayer wedge zones within such grains. Little of the naturally occurring Cs in the soil samples was extractable by chemical agents that would remove Cs from ordinary cation-exchange sites and from within non-silicate soil components. Furthermore, most of the natural Cs was inaccessible for isotope dilution under slightly acidic conditions approximating the natural soil environment. These observations support the idea that most of the Cs in these soils has become effectively fixed in the narrower parts of interlayer wedge zones. Control of Cs uptake and fixation by highly Csselective interlayer wedge sites would account for the large distribution coefficients found for 137Cs at the low aqueous Cs concentrations typical of environmental systems and also for the relatively large concentrations of stable Cs in the SRS soils.

Keywords

Hydroxy-interlayered VermiculiteInterlayer Wedge ZonesIsotope DilutionNatural CesiumRadiocesiumSavannah River SiteSoilSorption
Type
Article
Information
Clays and Clay Minerals , Volume 62 , Issue 3 , June 2014 , pp. 161 - 173
Copyright
Copyright © Clay Minerals Society 2014

Access options

Get access to the full version of this content by using one of the access options below. (Log in options will check for institutional or personal access. Content may require purchase if you do not have access.)

References

Barnhisel, R.I. Bertsch, P.M., Dixon, J.B. and Weed, S.B., 1989 Chlorites and hydroxy-interlayered vermiculite and smectite Minerals in Soil Environments 2nd edition Madison, Wisconsin, USA Soil Science Society of America 729–788.Google Scholar
Clark, S.B. Johnson, W.H. Malek, M.A. Serkiz, S.M. and Hinton, T.G., 1996 A comparison of sequential extraction techniques to estimate geochemical controls on the mobility of fission product, actinide, and heavy metal contaminants in soils Radiochimica Acta 74 173–179.CrossRefGoogle Scholar
Comans, R.N.J. and Hockley, D.E., 1992 Kinetics of cesium sorption on illite Geochimica et Cosmochimica Acta 56 1157–1164.CrossRefGoogle Scholar
Comans, R.N.J. Haller, M. and De Preter, P., 1991 Sorption of cesium on illite: Non-equilibrium behaviour and reversibility Geochimica et Cosmochimica Acta 55 433–440.CrossRefGoogle Scholar
Cremers, A. Elsen, A. De Preter, P. and Maes, A., 1988 Quantitative analysis of radiocaesium retention in soils Nature 335 247–249.CrossRefGoogle Scholar
Diesing, W.E. Sinaj, S. Sarret, G. Manceau, A. Flura, T. Demaria, P. Siegenthaler, A. Sappin-Didier, V. and Frossard, E., 2008 Zinc speciation and isotopic exchangeability in soils polluted with heavy metals European Journal of Soil Science 59 716–729.CrossRefGoogle Scholar
Dion, H.M. Romanek, C.S. Hinton, T.G. and Bertsch, P.M., 2005 Cesium-137 in floodplain sediments of the Lower Three Runs Creek on the DOE Savannah River Site Journal of Radioanalytical and Nuclear Chemistry 264 481–488.Google Scholar
Elprince, A.M. Rich, C.I. and Martens, D.C., 1977 Effect of temperature and hydroxy aluminum interlayers on the adsorption of trace radioactive cesium by sediments near water-cooled nuclear reactors Water Resources Research 13 375–380.CrossRefGoogle Scholar
Findley, M., 1998 Characterizing the environmental availability of trace metals in soils at the Savannah River Site M.S. thesis Clemson, South Carolina, USA Clemson University.Google Scholar
Goto, M., 2001 Development of a quantitative model for binding cesium to SRS soils M.S. thesis Atlanta, Georgia, USA Georgia Institute of Technology.Google Scholar
Goto, M. Rosson, R. Wampler, J.M. Elliott, W.C. Serkiz, S. and Kahn, B., 2008 Freundlich and dual Langmuir isotherm models for predicting 137Cs binding on Savannah River Site soils Health Physics 94 18–32.CrossRefGoogle ScholarPubMed
Grütter, A. von Gunten, H.R. Kohler, M. and Rössler, E., 1990 Sorption, desorption and exchange of cesium on glaciofluvial deposits Radiochimica Acta 50 177–184.CrossRefGoogle Scholar
Harris, W.G. Morrone, A.A. and Coleman, S.E., 1992 Occluded mica in hydroxy-interlayered vermiculite grains from a highly-weathered soil Clays and Clay Minerals 40 32–39.CrossRefGoogle Scholar
Harris, W.G. Hollien, K.A. Bates, S.R. and Acree, W.A., 1992 Dehydration of hydroxy-interlayered vermiculite as a function of time and temperature Clays and Clay Minerals 40 335–340.CrossRefGoogle Scholar
Jackson, M.L., 1969 Soil Chemical Analysis Advanced Course 2nd edition Madison, USA University of Wisconsin.Google Scholar
Kaplan, D.I. Sumner, M.E. Bertsch, P.M. and Adriano, D.C., 1996 Chemical conditions conducive to the release of mobile colloids from ultisol profiles Soil Science Society of America Journal 60 269–274.CrossRefGoogle Scholar
Kaplan, D.I. Bertsch, P.M. and Adriano, D.C., 1997 Mineralogical and physicochemical differences between mobile and nonmobile colloidal phases in reconstructed pedons Soil Science Society of America Journal 61 641–649.CrossRefGoogle Scholar
Karathanasis, A.D. and Hajek, B.F., 1982 Revised methods for rapid quantitative determination of minerals in soil clays Soil Science Society of America Journal 46 419–425.CrossRefGoogle Scholar
Karathanasis, A.D. Adams, F. and Hajek, B.F., 1983 Stability relationships in kaolinite, gibbsite, and Al-hydroxy interlayered vermiculite soil systems Soil Science Society of America Journal 47 1247–1251.CrossRefGoogle Scholar
Kirkland, D.L. and Hajek, B.F., 1972 Formula derivation of Al-interlayered vermiculite in selected soil clays Soil Science 114 317–322.CrossRefGoogle Scholar
Kunze, G.W. and Dixon, J.B., 1986 Pretreatment for mineralogical analysis Methods of Soil Analysis 2nd edition Madison, Wisconsin, USA American Society of Agronomy 91–99.Google Scholar
Lim, C.H. Jackson, M.L. Koons, R.D. and Helmke, P.A., 1980 Kaolins: Sources of differences in cation-exchange capacities and cesium retention Clays and Clay Minerals 28 223–229.CrossRefGoogle Scholar
Looney, B.B. Eddy, C.A. Ramsdeen, M. Pickett, J. Rogers, V. Scott, M.T. and Shirley, P.A., 1990 Geochemical and physical properties of soils and shallow sediments at the Savannah River Site WSRC-RP-90-1031, Westinghouse Savannah River Company South Carolina, USA Aiken.Google Scholar
Maes, E. Delvaux, B. and Thiry, Y., 1998 Fixation of radiocaesium in an acid brown forest soil European Journal of Soil Science 49 133–140.CrossRefGoogle Scholar
Meunier, A., 2007 Soil hydroxy-interlayered minerals: A reinterpretation of their crystallochemical properties Clays and Clay Minerals 55 380–388.CrossRefGoogle Scholar
Miller, W.P. Martens, D.C. and Zelazny, L.W., 1986 Effect of sequence in extraction of trace metal from soils Soil Science Society of America Journal 50 598–601.CrossRefGoogle Scholar
Nakao, A. Thiry, Y. Funakawa, S. and Kosaki, T., 2008 Characterization of the frayed edge site of micaceous minerals in soil clays influenced by different pedogenetic conditions in Japan and northern Thailand Soil Science and Plant Nutrition 54 479–489.CrossRefGoogle Scholar
Nakao, A. Funakawa, S. and Kosaki, T., 2009 Hydroxy-Al polymers block the frayed edge sites of illitic minerals in acid soils: studies in southwestern Japan at various weathering stages European Journal of Soil Science 60 127–138.CrossRefGoogle Scholar
Naumann, T.E. Elliott, W.C. and Wampler, J.M., 2012 K-Ar age constraints on the origin of micaceous minerals in Savannah River Site soils, South Carolina, USA Clays and Clay Minerals 60 496–506.CrossRefGoogle Scholar
NCRP, 2006 Cesium-137 in the environment: radioecology and approaches to assessment and management Bethesda, MD, National Council on Radiation Protection and Measurements; NCRP Report 154 .Google Scholar
Prout, W.E., 1958 Adsorption of radioactive waste by Savannah River Plant soil Soil Science 86 13–17.CrossRefGoogle Scholar
Rich, C.I. and Black, W.R., 1964 Potassium exchange as affected by cation size, pH, and mineral structure Soil Science 97 384–390.CrossRefGoogle Scholar
Rogers, V.A., 1990 Soil survey of Savannah River Plant area, parts of Aiken, Barnwell, and Allendale counties, South Carolina Washington, DC USDA Soil Conservation Service.Google Scholar
Ruhe, R.V. and Matney, E.A., 1980 Clay mineralogy of selected sediments and soils at the Savannah River Plant South Carolina Aiken.Google Scholar
Segall, M.P. Siron, D.L. and Colquhoun, D.J., 2000 Depos i t ional and diagenetic signatures of Late Eocene-Oligocene sediments, South Carolina Sedimentary Geology 134 27–47.CrossRefGoogle Scholar
Smolders, E. Brans, K. Földi, A. and Merckx, R., 1999 Cadmium fixation in soils measured by isotopic dilution Soil Science Society of America Journal 63 78–85.CrossRefGoogle Scholar
Wampler, J.M. Krogstad, E.J. Elliott, W.C. Kahn, B. and Kaplan, D.I., 2012 Long-term selective retention of natural Cs and Rb by highly weathered coastal plain soils Environmental Science & Technology 46 3837–3843.CrossRefGoogle ScholarPubMed