Parametric study of ternary ettringite-based systems for radwaste solidification and stabilization

Currently, there is a demand in furthering technological solutions to embed radioactive waste. A kind of this waste produced during the reprocessing of nuclear fuel is characterized by high pH sensitivity. Some organic matrixes (e.g. bitumen) developed to condition this waste are currently reconsidered by nuclear safety regulators. Therefore the cementation in ettringite systems might be a promising solution to solidify and stabilize this radioactive waste. Calcium Aluminate Cement (CAC) are planned to be used, instead of Ordinary Portland Cement (OPC), to form a significant amount of ettringite able to catch water molecules when forming. Moreover, due to the low pH of CAC-based matrixes, the latter have a good compatibility with the compounds used to stabilize active elements. However, the heat generated by hydration and the chemistry of waste require additional components. This paper details the investigations carried out on the CAC systems combined with Supplementary Cementing Materials. First theoretical studies show the main characteristics of reaction for the blends - especially: kinetics and type of hydrates formed, pH and chemistry of pore solution. Formulations are optimized to be in accordance with the stability of high pH sensitivity radioactive waste. Thereafter, parametric experiments including simulated waste are realized to study the rheological and the heat properties of the mixes. It appears that an increase in sulfate content ensures the formation and stability of ettringite and can greatly decrease the pH of pore solutions due to the formation of ettringite/AH₃ in a larger extent. Results show that increasing slag content in the CAC system reduces the heat generated during hydration and that the addition of quartz filler in simulated wastes has increased the nucleation surface