Abstract
As part of the homogeneous actinide recycling strategy, the EURO-GANEX process is one of the most promising options to achieve the goal of minor actinides recovery. Improvements made to EURO-GANEX system have resulted in the emergence of the so-called New EURO-GANEX process, where the composition of the solvent has been modified by replacing TODGA and DMDOHEMA with cis-mTDDGA in the organic phase and SO3-Ph-BTP with PyTri-Diol in the aqueous phase in order to resolve important issues. The objective of this work is 2-fold: evaluate the gamma radiolytic resistance of the new EURO-GANEX process by dynamic irradiation conditions simulating the three main steps of the process and validate the design of CIEMAT Náyade, CEA Marcel, and INL irradiation loop devices since each of them mimics different aspects of the real process. The Náyade and INL loops could irradiate the organic and aqueous phases together, whereas in the CEA loop, the irradiated solvent is recycled continuously inside a platform with several stages of mixer-settlers containing aqueous flows simulating the three main steps of the process. The extraction performances and changes in the composition of the solvent have been analyzed during the irradiation experiment by different techniques: gamma spectrometry and ICP-MS/OES for cations or radioactive tracer extraction and HPLC-MS to identify and quantify the degradation compounds. Despite some differences between the three irradiation facilities, this interinstitutional study shows that these three comparative tools provide similar trends in the radiolytic stability of a liquid-liquid extraction system. Favorable extraction results for the different steps are obtained according to the static irradiation studies found in literature. However, the degradation of cis-mTDDGA is appreciable leading to degradation compounds, some of which form precipitates and produce important changes in viscosity, important aspects that must be addressed prior to the successful industrial application of the new EURO-GANEX process.
| Original language | English |
|---|---|
| Pages (from-to) | 20326-20339 |
| Number of pages | 14 |
| Journal | Industrial and Engineering Chemistry Research |
| Volume | 62 |
| Issue number | 47 |
| DOIs | |
| State | Published - Nov 29 2023 |
Funding
The work carried out by CIEMAT was developed and funded under the framework of the European H2020 GENIORS Project (Contract no. 730227) and Spanish SYTRAD II project (National R&D program: “Retos de la Sociedad”, reference number: ENE2017-89280-R). The studies carried out in MARCEL loop test was funded by the CEA, Energy Division, Research Department on Mining and Fuel Recycling Processes, under contract EUR857755171. The experimental work conducted by D.R.P. at the Idaho National Laboratory was supported by the Nuclear Technology Research and Development Program, Office of Nuclear Energy, DOE Idaho Operations Office, under contract DE-AC07-05ID14517. The synthesis efforts by S.J.-P. at Oak Ridge National Laboratory were supported by the Nuclear Technology Research and Development Program, Office of Nuclear Energy, U.S. Department of Energy. A.C. and M.C.G. are grateful for the use of facilities acquired in the framework of the COMP-HUB and COMP-R initiative by the Departments of Excellence Program of MUR, Rome, Italy, 2018-2022 and 2023-2027.
| Funders | Funder number |
|---|---|
| Nuclear Technology Research and Development Program | |
| U.S. Department of Energy | |
| Office of Nuclear Energy | |
| Horizon 2020 Framework Programme | 730227, ENE2017-89280-R |
| Idaho Operations Office, U.S. Department of Energy | DE-AC07-05ID14517 |
| Commissariat à l'Énergie Atomique et aux Énergies Alternatives | EUR857755171 |