Microemulsions and Aggregation Formation in Extraction Processes for Used Nuclear Fuel: Thermodynamic and Structural Studies

Nilsson, Mikael¹ 

[1] Univ. of California, Irvine, CA (United States)

关键词: SOLVENT EXTRACTION;    TBP;    IONS;    METALS;    MICROEMULSIONS;    SPENT FUELS;    MATERIALS RECOVERY;    AGGLOMERATION;    PHOSPHORIC ACID;    MICELLAR SYSTEMS;    COMPLEXES;    CORRELATIONS;    EFFICIENCY;    CHEMICAL REACTION KINETICS;    LIGANDS;    P;   

DOI  :  10.2172/1258483
RP-ID  :  DOE/NEUP--11-3120
PID  :  OSTI ID: 1258483
Others  :  Other: 11-3120
Others  :  TRN: US1601511

学科分类：核能源与工程

美国|英语

来源: SciTech Connect

【 摘 要 】

Advanced nuclear fuel cycles rely on successful chemical separation of various elements in the used fuel. Numerous solvent extraction (SX) processes have been developed for the recovery and purification of metal ions from this used material. However, the predictability of process operations has been challenged by the lack of a fundamental understanding of the chemical interactions in several of these separation systems. For example, gaps in the thermodynamic description of the mechanism and the complexes formed will make predictions very challenging. Recent studies of certain extraction systems under development and a number of more established SX processes have suggested that aggregate formation in the organic phase results in a transformation of its selectivity and efficiency. Aggregation phenomena have consistently been interfering in SX process development, and have, over the years, become synonymous with an undesirable effect that must be prevented. This multiyear, multicollaborative research effort was carried out to study solvation and self-organization in non-aqueous solutions at conditions promoting aggregation phenomena. Our approach to this challenging topic was to investigate extraction systems comprising more than one extraction reagent where synergy of the metal ion could be observed. These systems were probed for the existence of stable microemulsions in the organic phase, and a number of high-end characterization tools were employed to elucidate the role of the aggregates in metal ion extraction. The ultimate goal was to find connections between synergy of metal ion extraction and reverse micellar formation. Our main accomplishment for this project was the expansion of the understanding of metal ion complexation in the extraction system combining tributyl phosphate (TBP) and dibutyl phosphoric acid (HDBP). We have found that for this system no direct correlation exists for the metal ion extraction and the formation of aggregates, meaning that the metal ion is not solubilized in a reverse micelle core. Rather we have found solid evidence that the metal ions are extracted and coordinated by the organic ligands as suggested by classic SX theories. However, we have challenged the existence of mixed complexes that have been suggested to exist in this particular extraction system. Most importantly we have generated a wealth of information and trained students on important lab techniques and strengthened the collaboration between the DOE national laboratories and US educational institution involved in this work.