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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
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
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Abstract

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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.

Type
Article
Copyright
Copyright © Clay Minerals Society 2014

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