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Diffusion of tritiated water and 22Na+ through non-degraded hardened cement pastes
Authors:Tits J  Jakob A  Wieland E  Spieler P
Institution:Waste Management Laboratory, Paul Scherrer Institute, CH-5232, Villigen PSI, Switzerland. jan.tits@psi.ch
Abstract:Diffusion experiments through hardened cement pastes (HCP) using tritiated water (HTO) and 22Na(+), considered to be conservative tracers, have been carried out in triplicates in a glove box under a controlled nitrogen atmosphere. Each experiment consisted of a through-diffusion test followed by an out-diffusion test. The experimental data were inversely modelled applying an automated Marquardt-Levenberg procedure. The analysis of the through-diffusion data allowed the extraction of values for the effective diffusion coefficients, D(e), and the rock capacity factor, alpha. Good agreement between measured and calculated tracer breakthrough curves was achieved using both a simple diffusion model without sorption and a diffusion/linear sorption model. The best-fit K(d)-values were found to be consistent with R(d)-values measured in previous batch-sorption experiments. The best-fit values from the through-diffusion tests were then used to predict the results of subsequent out-diffusion experiments. Good agreement between experimental data and predictions was achieved only for the case of linear sorption. Isotopic exchange can only partially account for both the amount of tracer taken up in the batch-sorption tests and the measured retardation in the diffusion experiments and, hence, additional mechanisms have to be invoked to explain the data.
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