Development of a TODGA based Process for Partitioning of Actinides from a PUREX Raffinate Part I: Batch Extraction Optimization Studies and Stability Tests

Разработка процесса на основе TODGA для разделения актинидов из раффината PUREX. Часть I: оптимизация пакетных экстракционных исследований и испытания на стабильность
Giuseppe Modolo, Hanna Asp, Christian Schreinemachers, H. Vijgen
2007-10-01

TODGATODGA + TBPactinides(III) and lanthanides(III) separationoxalic acid complexationradiolysis and hydrolysis stability
The extractant, N,N,N′,N′‐tetraoctyl diglycolamide (TODGA) has been evaluated for the separation of actinides(III) and lanthanides(III) from a high active raffinate (HAR). The effect of oxalic acid and HEDTA complexant on the extraction of actinides(III), lanthanides(III), and important fission products (e.g. Mo, Pd, Sr, Zr, Ru etc.) from synthetic HAR has been studied with 0.2 mol/L TODGA in TPH. With an extractant mixture of TODGA and tributyl phosphate (TBP) the amount of oxalic acid can be reduced to less than 0.3 mol/L for the effective complexation of zirconium, whereas the distribution ratios of actinides(III) and lanthanides(III) are still high for the separation from HAR. Furthermore the maximum loading of lanthanides (e.g. Nd) can be significantly increased by adding TBP to the extractant. However, the extraction of oxalic acid and nitric acid also increased by the addition of TBP, which can lead to problems during back extraction of the loaded extractant. Extraction studies after radiolysis and hydrolysis reveal that the TODGA+TBP mixture is a sufficient stable extraction system suited for further process development studies.
1
0.2 mol/L TODGA in TPH effectively extracts actinides(III) and lanthanides(III) from synthetic high active raffinate (HAR).
2
Adding TBP to TODGA allows reduction of required oxalic acid to <0.3 mol/L while effectively complexing zirconium and maintaining high An(III)/Ln(III) distribution ratios.
3
Addition of TBP increases extraction of oxalic acid and nitric acid, which can cause issues during back-extraction of loaded extractant.
4
Radiolysis and hydrolysis tests show the TODGA+TBP mixture is sufficiently stable for further process development.
5
TBP addition significantly increases maximum lanthanide (e.g., Nd) loading capacity of the extractant mixture.

TODGA-based solvent extraction system (0.2 mol/L TODGA in TPH, with/without TBP) for partitioning actinides(III) and lanthanides(III) from a high active raffinate (HAR)

Batch extraction performance and stability: effects of oxalic acid and HEDTA complexants, TBP addition on distribution ratios, metal loading (lanthanides like Nd), co-extraction of oxalic/nitric acid, and radiolysis/hydrolysis stability for actinide/lanthanide separation from PUREX raffinate

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2007-10-01
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Giuseppe Modolo
Hanna Asp
Christian Schreinemachers
H. Vijgen
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