Retardation of Chlorine-36 by Cementitious Materials Relevant to the Disposal of Radioactive Wastes

Abstract

The activation product chlorine-36 (36Cl) is an important radionuclide within the context of the disposal of nuclear wastes, due to its long half-life and environmental mobility. Its behaviour in a range of potential cementitious encapsulants and backfill materials was studied by evaluating its uptake by pure cement hydration phases and hardened cement pastes (HCP). Limited uptake of chloride was observed on calcium silicate hydrates (C-S-H) by electrostatic sorption and by calcium monosulphoferroaluminate hydrate (AFm) phases, due to anion exchange/solid solution formation. Diffusion of 36Cl through cured monolithic HCP samples, representative of cementitious materials considered for use in deep geological repositories across Europe, revealed a markedly diverse migration behaviour. Two of the matrices, a ground granulated blast furnace slag/ordinary Portland cement blend (GGBS–OPC) and an ordinary Portland cement (CEM I) effectively retarded 36Cl migration, retaining the radionuclide in narrow, reactive zones. The migration behaviour of 36Cl within the cementitious matrices is not strictly correlated to the measured sorption distribution ratios (Rd-values), suggesting that physical factors related to the microstructure can also have a distinct effect on diffusion behaviour. The findings have implications when selecting cementitious grouts and/or backfill materials for 36Cl-bearing radioactive wastes.