Gamma radiolytic stability of the novel modified diglycolamide 2,2′-oxybis(< /i>N< //i>,< /i>N< //i>-didecylpropanamide) (mTDDGA) for grouped actinide extraction

Verlinden, Bart; Van Hecke, Karen; Wilden, Andreas; Hupert, Michelle; Santiago-Schuebel, Beatrix; Egberink, Richard JM; Verboom, Willem; Kowalski, Piotr M; Modolo, Giuseppe; Verwerft, Marc; Binnemans, Koen; Cardinaels, Thomas

doi:10.1039/d1ra08761d

Gamma radiolytic stability of the novel modified diglycolamide 2,2′-oxybis(< /i>N< //i>,< /i>N< //i>-didecylpropanamide) (mTDDGA) for grouped actinide extraction

Author:

Verlinden, Bart

Van Hecke, Karen ; Wilden, Andreas ; Hupert, Michelle ; Santiago-Schuebel, Beatrix ; Egberink, Richard JM ; Verboom, Willem ; Kowalski, Piotr M ; Modolo, Giuseppe ; Verwerft, Marc ; Binnemans, Koen ; Cardinaels, Thomas

Keywords:

Science & Technology, Physical Sciences, Chemistry, Multidisciplinary, Chemistry, RADIATION-CHEMISTRY, FISSION-PRODUCTS, NITRIC-ACID, SEPARATION, SOLVENT, DEGRADATION, TODGA, COMPLEXATION, HYDROLYSIS, PLUTONIUM, 03 Chemical Sciences, 34 Chemical sciences

Abstract:

Reprocessing of spent nuclear fuel aims at improving resource efficiency and reducing its radiotoxicity and heat production in the long term. The necessary separation of certain metal ions from the spent fuel solutions can be achieved using different solvent extraction processes. For the scenario of the EURO-GANEX process, the use of the new, modified diglycolamide 2,2'-oxybis(N,N-didecylpropanamide) (mTDDGA) was recently proposed to simplify the current solvent composition and reduce extraction of fission products. Before further developing the process based on this new ligand, its stability under ionizing radiation conditions needs to be studied. For this reason, gamma irradiation experiments were conducted followed by analyses with high performance liquid chromatography coupled to a mass spectrometer (HPLC-MS). The determined degradation rate of mTDDGA was found to be lower than that of the reference molecule N,N,N',N'-tetra-n-octyl-diglycolamide (TODGA). Many identified degradation compounds of both molecules are analogues showing the same bond breaking, although also unreported de-methylation, double/triple de-alkylation and n-dodecane addition products were observed.