DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Interinstitutional Study of the New EURO-GANEX Process Resistance by Gamma Irradiation Test Loops

Journal Article · · Industrial and Engineering Chemistry Research
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [3];  [3]; ORCiD logo [4]; ORCiD logo [5]; ORCiD logo [5]; ORCiD logo [6]; ORCiD logo [7]
  1. Research Centre for Energy, Environment and Technology (CIEMAT), Madrid (Spain)
  2. Alternative Energies and Atomic Energy Commission (CEA), (France); Montpellier University (France)
  3. Idaho National Laboratory (INL), Idaho Falls, ID (United States)
  4. Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
  5. Univ. of Parma (Italy)
  6. Forschungszentrum Julich (Germany). Inst. fur Energie- und Klimaforschung (IEK)
  7. Karlsruhe Inst. of Technology (KIT) (Germany). Institute for Nuclear Waste Disposal (INE)

As part of the homogeneous actinides recycling strategy, the EURO-GANEX process is one of the most promising options to achieve the goal of minor actinides recovery. However, EURO-GANEX also has various drawbacks that are being addressed. 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 twofold: evaluate the gamma radiolysis 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. Náyade and the INL loops could irradiate together the organic and aqueous phases, 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 analysed during the irradiation experiment by different techniques: gamma spectrometry and ICP-MS/OES for cations or tracers extraction, and HPLC-MS to quantify the degradation and evaluate the degradation compounds. Additionally, in spite of some differences between the three-irradiation facilities, this inter-institutional study shows that they are three comparative tools, which provide results on the stability towards radiolysis of a liquid-liquid extraction system. Favourable 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.

Research Organization:
Idaho National Laboratory (INL), Idaho Falls, ID (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Organization:
USDOE Office of Nuclear Energy (NE)
Grant/Contract Number:
AC07-05ID14517
OSTI ID:
2282761
Report Number(s):
INL/JOU--23-73547-Rev001
Journal Information:
Industrial and Engineering Chemistry Research, Journal Name: Industrial and Engineering Chemistry Research Journal Issue: 47 Vol. 62; ISSN 0888-5885
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English

References (43)

Radiolytic effects on Actinide complexation with a hydrophilic PyTri ligand journal February 2021
Selective actinide(III) separation using 2,6-bis[1-(propan-1-ol)-1,2,3-triazol-4-yl]pyridine (PyTri-Diol) in the innovative-SANEX process: laboratory scale counter current centrifugal contactor demonstration journal April 2022
Development of experimental irradiation strategies to evaluate the robustness of TODGA and water-soluble BTP extraction systems for advanced nuclear fuel recycling journal December 2020
THE NOVEL EXTRACTANTS, DIGLYCOLAMIDES, FOR THE EXTRACTION OF LANTHANIDES AND ACTINIDES IN HNO 3n -DODECANE SYSTEM journal January 2001
A review of separation processes proposed for advanced fuel cycles based on technology readiness level assessments journal November 2019
Hydrophilic Clicked 2,6-Bis-triazolyl-pyridines Endowed with High Actinide Selectivity and Radiochemical Stability: Toward a Closed Nuclear Fuel Cycle journal May 2016
An overview of solvent extraction processes developed in Europe for advanced nuclear fuel recycling, Part 2 — homogeneous recycling journal November 2021
Modified Diglycolamides for the An(III) + Ln(III) Co-separation: Evaluation by Solvent Extraction and Time-Resolved Laser Fluorescence Spectroscopy journal January 2014
N,N,N′,N′‐Tetraoctyl Diglycolamide (TODGA): A Promising Extractant for Actinide‐Partitioning from High‐Level Waste (HLW) journal July 2005
Actinide(III)/Lanthanide(III) Separation Via Selective Aqueous Complexation of Actinides(III) using a Hydrophilic 2,6-Bis(1,2,4-Triazin-3-Yl)-Pyridine in Nitric Acid journal August 2012
Development of a gamma irradiation loop to evaluate the performance of a EURO-GANEX process journal May 2022
Improving the nuclear energy sustainability by decreasing its environmental footprint. Guidelines from life cycle assessment simulations journal September 2016
An overview of solvent extraction processes developed in Europe for advanced nuclear fuel recycling, part 1 — heterogeneous recycling journal July 2020
Behaviour of the extractant Me-TODGA upon gamma irradiation: quantification of degradation compounds and individual influences on complexation and extraction journal January 2017
Distribution of plutonium, americium and interfering fission products between nitric acid and a mixed organic phase of TODGA and DMDOHEMA in kerosene, and implications for the design of the “EURO-GANEX” process journal February 2015
Development of a TODGA based Process for Partitioning of Actinides from a PUREX Raffinate Part I: Batch Extraction Optimization Studies and Stability Tests journal October 2007
Studies on hydrolysis and radiolysis of N,N,N′,N′-tetraoctyl-3-oxapentane-1,5-diamide journal January 2002
Radiolytic Stability of TODGA: Characterization of Degraded Samples under Different Experimental Conditions journal January 2012
Radiolysis study of actinide complexing agent by irradiation with helium ion beam journal December 2009
Gamma radiolytic stability of the novel modified diglycolamide 2,2′-oxybis(N,N-didecylpropanamide) (mTDDGA) for grouped actinide extraction journal January 2022
Partitioning and transmutation strategy R&D for nuclear spent fuel: the SACSESS and GENIORS projects journal January 2020
Solvent Optimization Studies for a New EURO-GANEX Process with 2,2’-Oxybis(N,N-di-n-decylpropanamide) (mTDDGA) and Its Radiolysis Products journal October 2022
Modified diglycolamides for grouped actinide separation journal November 2017
A Comparison of the γ -Radiolysis of TODGA and T(EH)DGA Using UHPLC-ESI-MS Analysis journal March 2015
A Study of the γ-Radiolysis of N,N -Didodecyl- N′,N′ -Dioctyldiglycolamide Using UHPLC-ESI-MS Analysis journal June 2016
Gamma Radiolysis of TODGA and CyMe 4 BTPhen in the Ionic Liquid Tri- n -Octylmethylammonium Nitrate journal January 2020
Time-Resolved Laser Fluorescence Spectroscopy Study of the Coordination Chemistry of a Hydrophilic CHON [1,2,3-Triazol-4-yl]pyridine Ligand with Cm(III) and Eu(III) journal February 2017
Radiolytic and hydrolytic degradation of the hydrophilic diglycolamides journal June 2018
Effects of Gamma Irradiation on the Extraction Properties of Innovative Stripping Solvents for i-SANEX/GANEX Processes journal July 2021
Synthesis and Am/Eu extraction of novel TODGA derivatives journal August 2010
Optimization and Single-Stage Centrifugal Contactor Experiments with the Novel Hydrophilic Complexant PyTri-Diol for the i -SANEX Process journal June 2018
Stability studies of GANEX system under different irradiation conditions journal January 2019
Radiolytic degradation of hydrophilic PyTri ligands for minor actinide recycling journal September 2019
Plutonium Loading of Prospective Grouped Actinide Extraction (GANEX) Solvent Systems based on Diglycolamide Extractants journal March 2012
Dosimetry and methodology of gamma irradiation for degradation studies on solvent extraction systems journal November 2020
The EURO-GANEX Process: Current Status of Flowsheet Development and Process Safety Studies journal January 2016
Gamma radiolysis of hydrophilic diglycolamide ligands in concentrated aqueous nitrate solution journal January 2019
Assessment of the environmental footprint of nuclear energy systems. Comparison between closed and open fuel cycles journal May 2014
Homogenous recycling of transuranium elements from irradiated fast reactor fuel by the EURO-GANEX solvent extraction process journal May 2019
Gamma-radiolytic stability of new methylated TODGA derivatives for minor actinide recycling journal January 2015
The applications of formo- and aceto-hydroxamic acids in nuclear fuel reprocessing journal June 1998
Diamex Process for Minor Actinide Partitioning: Hydrolytic and Radiolytic Degradations of Malonamide Extractants journal June 2001
Unprecedented Inversion of Selectivity and Extraordinary Difference in the Complexation of Trivalent f  Elements by Diastereomers of a Methylated Diglycolamide journal March 2019