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Behaviour of the extractant Me-TODGA upon gamma irradiation: quantification of the degradation compounds and individual influences on complexation and extraction

Abstract

Diglycolamides (DGAs), and in particular N,N,N’,N’-tetraoctyl diglycolamide (TODGA), are well-known candidates for the co-extraction of trivalent actinides (An(III)) and lanthanides (Ln(III)) from highly acidic aqueous solutions of nuclear waste. A derivative of TODGA, the so-called Me-TODGA with the addition of a methyl-substituent on the central part of the TODGA molecule, has been proposed to improve its stability properties and extracting behaviour. This work describes the stability and viability of Me-TODGA by studying the properties of its degradation compounds formed upon gamma irradiation. The main degradation products have been synthesised and studied individually. Particular attention has been paid on their quantification, as well as complexing and extracting properties, for a better understanding of the degradation pathways and the behaviour of the solvents upon gamma irradiation. The extraction behaviour of the irradiated Me-TODGA solvents and its degradation compounds have been studied toward the fission products and lanthanides present in a highly active raffinate (HAR) solution. Binding properties of the parent molecules (TODGA and Me-TODGA) and their main degradation compounds with Ln(III) have also been determined in homogeneous phase. All the results obtained on degradation compounds are compared with those of the parent molecules in order to assess the effects of these compounds on the separation process. Among the radiolytic compounds, 2-hydroxyoctylamides are the most problematic compounds because of their high affinity to lanthanides but also to other fission products.

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Publication details

The article was received on 14 Jun 2017, accepted on 28 Sep 2017 and first published on 29 Sep 2017


Article type: Paper
DOI: 10.1039/C7NJ02136D
Citation: New J. Chem., 2017, Accepted Manuscript
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    Behaviour of the extractant Me-TODGA upon gamma irradiation: quantification of the degradation compounds and individual influences on complexation and extraction

    V. Hubscher-Bruder, V. Mogilireddy, S. Michel, A. Leoncini, J. Huskens, W. Verboom, H. Galan, A. Núñez Gómez-Aleixandre, J. Cobos Sabate, G. Modolo, A. Wilden, H. Schmidt, M. Charbonnel, P. Guilbaud and N. Boubals, New J. Chem., 2017, Accepted Manuscript , DOI: 10.1039/C7NJ02136D

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