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The Use of Laboratory Adsorption Data and Models to PredictRadionuclide Releases from a Geological Repository: a BriefHistory

Published online by Cambridge University Press:  03 September 2012

Donald Langmuir
Donald Langmuir*
Affiliation:
U.S. Nuclear Waste Technical Review Board 1100 Wilson Boulevard, Suite 910, Arlington, VA 22209
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Abstract

Radionuclide (RN) adsorption has long been recognized as important to assurethe isolation of nuclear wastes in a geological repository [1]. Laboratorymeasured RN adsorption data have generally been expressed as distributioncoefficient (Kd) values or adsorption isotherms. The properapplication of these models is to site conditions nearly identical to thoseused in the laboratory adsorption experiments. This has required thatmultiple Kd's and isotherms be determined in a wide range ofexperiments designed to bracket expected repository conditions.

The surface complexation (SC) adsorption models were introduced in the late1970's. The best known of these models incorporate electrical double layer(EDL) theory [2]. Their use requires that the water chemistry and surfaceproperties of adsorbing rocks and minerals be fully characterized.Adsorption is then studied as reactions involving specific aqueous RNspecies (often complexes) and specific surface sites. Because the SC modelsare relatively mechanistic, they may allow extrapolation of adsorptionresults to repository conditions that lie outside the limited experimentalrange used to parameterize a given model. Turner [3] has shown that thediffuse layer model (the simplest SC model) fits a wide range of RNadsorption data as well as the more complex models. Others have suggestedways to generalize and estimate SC model parameters for a variety ofminerals, rocks and engineered materials (cf. [4,5,6,7,8,9,10,11,12].Degueldre and Werlni [12] and Degueldre et al. [13] have proposed asimplified SC model for RN adsorption that avoids EDL theory, in which theadsorption of RN species is estimated from linear free energyrelationships.

It is appropriate to ask how accurately RN adsorption behavior must be knownor understood for total system performance analysis (TSPA). In mostgeological settings now being considered for repository developmentglobally, it may suffice to select bounding Kd values for thedifferent rock types (cf. [14,15]). Use of the SC models to describe RNadsorption can provide us with increased confidence that minimum Kd's and the distribution of Kd values we mightpropose for TSPA are in fact conservative.

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Type
Research Article
Information
MRS Online Proceedings Library (OPL) , Volume 465: Symposium II – Scienfific Basis for Nuclear Waste Management XX , 1996 , 769
Copyright
Copyright © Materials Research Society 1997

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