Verlinden Bart, Van Hecke Karen, Wilden Andreas, Hupert Michelle, Santiago-Schübel Beatrix, Egberink Richard J M, Verboom Willem, Kowalski Piotr M, Modolo Giuseppe, Verwerft Marc, Binnemans Koen, Cardinaels Thomas
Belgian Nuclear Research Centre (SCK CEN), Institute for Nuclear Materials Science Boeretang 200 2400 Mol Belgium
Department of Chemistry, KU Leuven Celestijnenlaan 200F, P.O. Box 2404 3001 Leuven Belgium.
RSC Adv. 2022 Apr 25;12(20):12416-12426. doi: 10.1039/d1ra08761d. eCollection 2022 Apr 22.
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(,-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 ,,','-tetra--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 -dodecane addition products were observed.
乏核燃料后处理旨在提高资源利用效率,并从长远来看降低其放射性毒性和产热。通过不同的溶剂萃取工艺可以实现从乏燃料溶液中分离某些金属离子的必要操作。对于欧洲镧系元素分组萃取流程(EURO-GANEX)的情况,最近有人提议使用新型改性二甘醇酰胺2,2'-氧双(N,N'-二癸基丙酰胺)(mTDDGA)来简化当前的溶剂组成并减少裂变产物的萃取。在基于这种新配体进一步开发该流程之前,需要研究其在电离辐射条件下的稳定性。因此,进行了伽马辐照实验,随后采用高效液相色谱-质谱联用仪(HPLC-MS)进行分析。结果发现,mTDDGA的降解速率低于参考分子N,N,N',N'-四(2-乙基己基)二甘醇酰胺(TODGA)。尽管还观察到了未报道的去甲基化、双/三去烷基化和十二烷加成产物,但两种分子的许多已鉴定降解化合物都是显示相同键断裂的类似物。