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

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 âˆ¼ -14.9 kJ‧mol-1 and -8.03 âˆ¼ -12.4 kJ‧mol-1. And the calculated values of enthalpy change and entropy change are -18.8 âˆ¼ -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.

Study on the uranium (U(⠥)) adsorption stability of high-dose γ-ray-irradiated clay.

The Alxa region (Inner Mongolia, China) is one of the areas preselected for use as a geological repository of high-level radioactive waste in China. Radioactive waste produces radioactive rays during long-term storage, and the cumulative absorbed dose in 1000 years can significantly exceed the maximum of 0.7 MGy, thereby challenging the long-term adsorption stability of clay. This study employed 60Co gamma (γ)-rays to irradiate clay in air under a dose rate of 10 kGy/h. The changes in the internal structure and mechanisms of clay under different gamma radiation doses (1, 2, and 3 MGy) were investigated. Additionally, the adsorption properties of irradiated clay for U(Ⅵ) were tested under different conditions. The clay samples underwent minimal structural changes following high-dose irradiation, and the interlayer spacing was altered due to the fractured framework, dehydroxylation, and radiolysis of water. After irradiation, the Fe (Ⅱ) content in clay was significantly increased, unlike Fe (Ⅲ) content. The adsorption mechanisms of clay before and after the experiments were verified, revealing that the adsorption capacity of irradiated clay to U(Ⅵ) is reduced.

(Ce-Al)-oxide pillared bentonite: A high affinity sorbent for plutonium.

The ability of bentonite and montmorillonite pillared by Al-oxide and mixed (Ln-Al)-oxides (Ln = La, Ce) to remove 239plutonium solution species from water is comparatively investigated at pH 7 and pH 4. Small-angle scattering and neutron contrast variation with H2O/D2O mixtures is used to verify the ingress of water in the calcined products after hydrophilicity was introduced by an NH3-H2O vapor treatment. The size and shape of the (La/Ce)-Al oxo-hydroxy pillaring cations (2 nm spheres) is determined by small-angle x-ray scattering from the pillaring solutions. Not all of the oxide pillars improved Pu uptake compared with sodium montmorillonite. At neutral and acidic pH only (Ce-Al)-oxide pillared clays showed the ability to remove Pu over the concentration range studied (1.35 × 10-8-8 × 10-8 mol dm-3) with distribution coefficient (KD) values >104. XPS analysis of the (Ce-Al)-oxide pillared clays indicates the presence of Ce4+ as cerium dioxide. The progressive improvement in sorption performance in the order of pillar type Al2O3 < La2O3-Al2O3 << CeO2-Al2O3 reflects the increasing access of Pu solution species to the clay mineral layers by changes to the basal spacing and specific surface area, and also to the higher stability of the (Ce-Al)-oxide pillars.