Reproducibility of the uptake of U(VI) onto degraded cement pastes and calcium silicate hydrate phases

Abstract

AbstractThe U(VI) uptake in degraded cement pastes was undertaken in the laboratories of CEA/L3MR and SUBATECH in order to check the reproducibility of the study. Two well hydrated cement pastes, CEM I (Ordinary Portland Cement, OPC) and CEM V (blast furnace slag (BFS) and fly ash added to OPC) were degraded using similar protocols. Equilibrium solutions and solid materials were characterised for three degradation states for each paste. All samples are free of portlandite and the pH of the equilibrated cement solutions vary in the range 9.8-12.2. Three calcium silicate hydrate phases (C-S-H) were synthesised in order to compare the sorption properties of degraded cement pastes and of hydrate phases in similar pH conditions. In order to avoid precipitation processes, the operational solubility limit was evaluated before batch experiments. These solubility values vary significantly in the pH range [9-13] with a 2.4×10-7mol L-1minimum at pH close to 10.5. In batch sorption experiments, the distribution ratioRdvalues are high: 3×104-1.5×105mL g-1. The uptake of U(VI) increases when comparing the least and the most degraded cement pastes whereas the initial composition of cement has relatively insensitive effect. Sorption isotherms, expressed as a log[U(VI)solid]/log [U(VI)solution] plots are linear. A slope of 1 is calculated indicating the predominance of sorption processes. As sorption and desorption values are close, the uptake mechanism seems reversible. TheRdvalues measured in C-S-H suspensions are in good agreement withRdvalues of degraded cement pastes, and C-S-H materials could be one of the cementitious phases which control U(VI) uptake in cement pastes.