Use of Polyaminocarboxylic Acids as Hydrophilic Masking Agents for Fission Products in Actinide Partitioning Processes

Abstract

During the partitioning of trivalent actinides from High Active Raffinate (HAR) solutions, most processes have to cope with an undesirable co-extraction of some of the fission products. Four hydrophilic complexing agents of the group of polyaminocarboxylic acids, namely EDTA, HEDTA, DTPA, and CTDA were tested and compared for their ability to complex fission products in a simulated PUREX raffinate solution, thereby preventing their extraction into an organic solvent. Several solvents, based on TODGA and the DIAMEX reference molecule DMDOHEMA, that are commonly known to show quite high Zr and Pd co-extraction, were studied. Our investigations ultimately resulted in a substitution of oxalic acid and HEDTA by cyclohexanediaminetetraacetic acid (CDTA). A small addition of this hydrophilic complexing agent to the feed decreased the distribution ratios of Zr from 100 to <0.01. The suppression of Pd was also very effective, resulting in >90% of the metal retained in the feed solution. The extraction of trivalent actinides and lanthanides was not negatively affected by the presence of CDTA. Furthermore, experiments with high concentrations of Zr proved the applicability of this new masking agent. The suppression of Zr and Pd extraction was also verified at a high Pu loading which makes CDTA as a masking agent attractive for grouped actinide extraction processes (GANEX) as well as DIAMEX-SANEX type separations.

Keywords:

• Oxalic acid
• CDTA
• EDTA
• DTPA
• HEDTA
• TODGA
• DMDOHEMA
• solvent extraction
• Pd complexation
• Zr complexation
• GANEX

ACKNOWLEDGMENTS

Financial support for this research was provided by the European Commission (project ACSEPT – Contract No. FP7-CP-2007-211 267) and the German Federal Ministry of Education and Research (Contract No. 02NUK012E).