N,N,N’,N’-tetraethyldiglycolamide (TEDGA) is used in the French EXAm (extraction of americium) process to separate Am(III) from Cm(III) and Ln(III). In this study, the complexation behavior of TEDGA towards actinides(III) and lanthanides(III) was compared to its methyl-substituted derivatives Me-TEDGA and Me2-TEDGA under experimental conditions applying to the EXAm process. Using the EXAm solvent, 0.6 mol/L N,N’-dimethyl-N,N’-dioctyl-hexylethoxymalonamide (DMDOHEMA) and 0.45 mol/L bis(2-ethylhexyl)-phosphoric acid (HDEHP), An(III) and Ln(III) distribution ratios increase in the order TEDGA < Me-TEDGA < Me2-TEDGA. This is explained by differences in the strength of complexation in the aqueous phase: Conditional stability constants for the formation of [Cm(DGA)x]3+ complexes decrease in the order TEDGA > Me-TEDGA > Me2-TEDGA, as shown by time-resolved laser fluorescence spectroscopy (TRLFS). TRLFS measurements verified the exclusive existence of [Cm(DGA)3]3+ complexes in the aqueous phase. Both the homoleptic [Cm(DMDOHEMA)n]3+ and the heteroleptic [Cm(DGA)x(DMDOHEMA)y]3+ complexes were detected in the organic phase, as postulated in the literature.[1]
24 June 2021 in Journal of Radioanalytical and Nuclear Chemistry
Radioactive mercury waste constitutes a significant challenge, as no approved disposal concept yet exists for such waste in Germany. This work describes a decontamination and measurement procedure for a possible clearance of mercury from nuclear facilities and release into reuse or conventional hazardous waste disposal to reduce the amount of mercury in a nuclear repository. The measurement setup and procedure were developed and evaluated including Monte-Carlo N-Particle® Transport Code (MCNP® and Monte Carlo N-Particle® are registered trademarks owned by Los Alamos National Security, LLC, manager and operator of Los Alamos National Laboratory, (Werner 2018, Werner 2017)), simulations to ensure conservative assumptions during the measurements. Results from decontaminated mercury samples show that a clearance pursuant to the German regulations would be feasible.