Radial diffusion of radiocaesium and radioiodide through cementitious backfill

Abstract

The function of the backfill material in a geological disposal facility (GDF) is to chemically condition the environment of the near field and thereby chemically retard the transport of the radionuclides present in the waste. This function of the backfill material is usually referred to as chemical containment. Diffusion experiments are being carried out over periods up to four years to assess the diffusion of Cs, Ni, Eu, Th, U and I (as I−) through Nirex Reference Vault Backfill (NRVB). The method uses cylinders of NRVB (40mm diameter, 40–45mm height) which can be doped via a central well with the radionuclides of interest. Diffusion occurs radially into a surrounding solution already pre-equilibrated with the cement. This paper shows the results obtained during the first two years for experiments undertaken using 137Cs and 125I− tracers with and without carrier. Comparison is made to tritiated water under identical experimental conditions. Breakthrough of Cs and I− occurred within the first week of the experiments, reaching steady state in the surrounding solution after 20–50days. The maximum concentrations expected from the original inventories based on a simple dilution calculation have not been reached, indicating that retention in the matrix has occurred; ranging from 10% to 40% for Cs, and up to 50% for I−. Corresponding experiments using a solution containing cellulose degradation products (CDP) showed an increased diffusion for both Cs and I. Migration profiles have been obtained and the relative retention of each radionuclide has been confirmed using digital autoradiography. The results indicate that, for both isotopes, migration occurs through the cement matrix rather than through microfissures. However, whereas Cs is homogeneously distributed within the blocks, there is evidence of zones of preferential I− accumulation even where concentrations in solution have reached steady state. Transport modelling using GoldSim has replicated experimental observations, producing comparable partition ratios (Rd) to those reported in the literature.