Barium and Radium Complexation with Ethylenediaminetetraacetic Acid in Aqueous Alkaline Sodium Chloride Media

Abstract

The speciation of Ra2+ and Ba2+ with EDTA was investigated at 25 °C in aqueous alkaline NaCl media as a function of ionic strength (0.2–2.5 mol·L−1) in two pH regions where the EDTA4− and HEDTA3− species dominate. The stability constants for the formation of the [BaEDTA]2− and [RaEDTA]2− complexes were determined using an ion exchange method. Barium-133 and radium-226 were used as radiotracers and their concentrations in the aqueous phase were measured using liquid scintillation counting and gamma spectrometry, respectively. The specific ion interaction theory (SIT) was used to account for [NaEDTA]3− and [NaHEDTA]2− complex formation, and used to extrapolate the logarithms of the apparent stability constants (log10K) to zero ionic strength (BaEDTA2−: 9.86 ± 0.09; RaEDTA2−: 9.13 ± 0.07) and obtain the Ba2+ and Ra2+ ion interaction parameters: [ε(Na+, BaEDTA2−) = − (0.03 ± 0.11); ε(Na+, RaEDTA2−) = − (0.10 ± 0.11)]. It was found that in the pH region where HEDTA3− dominates, the reaction of Ba2+ or Ra2+ with the HEDTA3− ligand also results in the formation of the BaEDTA2− and RaEDTA2− complexes (as it does in the region where the EDTA4− ligand dominates) with the release of a proton. Comparison of the ion interaction parameters of Ba2+ and Ra2+ strongly indicates that both metal ions and their EDTA complexes have similar activity coefficients and undergo similar short-range interactions in aqueous NaCl media.