Stability of Eu(III)-silicate colloids: Effect of Eu content, pH, electrolyte and fulvic acid

Dissolved silicic acid in the environment has strong affinity for actinides (An), but An(III)-silicate colloids have been scarcely investigated. In this study, Eu(III)-silicate colloids, an analogue to An(III)-silicate, were prepared and the aggregation kinetics of the colloids was investigated as a function of Eu content (Si/Eu molar ratio), pH, background electrolyte (NaCl, NaNO₃, NaClO₄, KCl and CsCl) and fulvic acid (FA). Results indicated that the colloids with higher Si/Eu molar ratio exhibited higher stability under the same conditions. The stability of the colloids increased with increasing aqueous pH (7.1-9.4) and decreasing ionic strength, and the inhibition effect of monovalent electrolytes on the colloid stability followed the order of Na⁺ < K⁺ < Cs⁺ and Cl^- < NO₃^- < ClO₄^-. In addition, the presence of FA significantly increased the stability of the colloids. The dependence of the stability on the chemical conditions in all cases could be illustrated by DLVO theory. Disaggregation kinetics showed that the aggregation process of the colloids was not fully reversible, because a time-dependent size memory effect led to a bigger mean size of disaggregated colloids as compared to the initial ones. The present work provides detailed insight in the formation and stability of An(III)-silicate colloids under the alkaline conditions relevant to geological disposal of radioactive waste, which is critical for understanding the behavior of this type of colloids in the environment.