The mechanism and behavior of cesium adsorption from aqueous solutions onto carbonated cement slurry powder

Abstract

In this study, microstructural differences and changes in the adsorption capacity of cesium between cement and carbonated cement were investigated. Cement blocks were ground to powder for rapid carbonation, and microscopic variations were characterized by XRF, XRD, FT-IR, SEM, BET, and TGA. The characterization results show that the conversion of Ca(OH)2 and calcium silicate hydrate (C–S–H) gel to CaCO3 in cement after carbonation. And the component of Ca(OH)2 in the powder sample disappeared after three days of rapid carbonation. Batch experiments were used to investigate adsorption under the influence of time, initial cesium concentration, temperature, and ion coexistence. Pseudo-second-order kinetic and Langmuir isothermal model fitting could better describe the adsorption process and the results show that the maximum adsorption capacity of cement after carbonation surges from 29.6 μg‧g−1 to 1.58–5.89 mg‧g−1. (Different carbonating times lead to varying adsorption capacity.) The adsorption capacity decreases with increasing temperature. At temperatures of 293 K and 333 K, the calculated Gibbs free energy change values of cement with different carbonated degrees adsorbing cesium are −10.3 ∼ −14.9 kJ‧mol−1 and -8.03 ∼ −12.4 kJ‧mol−1. And the calculated values of enthalpy change and entropy change are −18.8 ∼ −23.8 kJ‧mol−1 and –27.9 ∼ –37.1 J‧mol−1‧K−1. Combining the characterization and adsorption results, the huge increase in cesium adsorption capacity is closely related to the conversion of Ca(OH)2 to CaCO3, which will provide a new perspective on the adsorption mechanism of cesium in cement.