Browse > Article
http://dx.doi.org/10.1016/j.net.2021.11.024

Development of a gamma irradiation loop to evaluate the performance of a EURO-GANEX process  

Sanchez-Garcia, I. (Centro de Investigaciones Energeticas, Medioambientales y Tecnologicas (CIEMAT))
Galan, H. (Centro de Investigaciones Energeticas, Medioambientales y Tecnologicas (CIEMAT))
Nunez, A. (Centro de Investigaciones Energeticas, Medioambientales y Tecnologicas (CIEMAT))
Perlado, J.M. (Universidad Politecnica de Madrid (UPM), Instituto de Fusion Nuclear)
Cobos, J. (Centro de Investigaciones Energeticas, Medioambientales y Tecnologicas (CIEMAT))
Publication Information
Nuclear Engineering and Technology / v.54, no.5, 2022 , pp. 1623-1634 More about this Journal
Abstract
A new irradiation loop design has been developed, which provides the ability to carry out radiolytic resistance studies of extraction systems simulating process relevant conditions in an easy and simple way. The step-by-step loop configuration permits an easy modification of settings and has a relative low volume requirement. This irradiation loop has been initially set up to test the main EURO-GANEX process steps: the lanthanide (Ln) and actinide (An) co-extraction followed by the transuranic (TRU) stripping. The performance and changes in the composition have been analyzed during the irradiation experiment by different techniques: gamma spectroscopy and ICP-MS for the extraction and corrosion behavior of the full system, and HPLC-MS and Raman spectroscopy to determine the degradation of the organic and aqueous solvents, respectively. The Ln and An co-extraction step and the corrosion that occurred during the first irradiation step revealed the favorable expected results according to literature. The effects of acidity changes occurred during the irradiation process, the presence of stainless corrosion products in solution as well as the new possible degradation compounds have been explored in the An stripping step. The results obtained demonstrate the importance of developing realistic irradiation experiments where different factors affecting the performance can be easily studied and isolated.
Keywords
Irradiation loop; EURO-GANEX process; Dynamic gamma irradiation; Solvent extraction; $TODGA+DMDOHEMA/SO_3-Ph-BTP$; Minor actinides; Reprocessing;
Citations & Related Records
Times Cited By KSCI : 1  (Citation Analysis)
연도 인용수 순위
1 H. Galan, D. Munzel, A. Nunez, U. Mullich, J. Cobos, A. Geist, In Stability and recyclability of SO3-Ph-BTP for i-SANEX process development, in: Proceedings of the International Solvent Extraction Conference (ISEC 2014), 2014, pp. 137-143.
2 H. Fricke, E.J. Hart, The Oxidation of Fe++ to Fe+++ by the irradiation with X-Rays of solutions of ferrous sulfate in sulfuric acid, J. Chem. Phys. 3 (1) (1935) 60-61.   DOI
3 I. Sanchez-Garcia, L.J. Bonales, H. Galan, J.M. Perlado, J. Cobos, Spectroscopic study of acetohydroxamic acid (AHA) hydrolysis in the presence of europium. Implications in the extraction system studies for lanthanide and actinide separation, New J. Chem. 43 (39) (2019) 15714-15722.   DOI
4 J. de Mendoza, B. Camafort, A.G. Espartero, A. Nunez, H. Galan, TODGA Industrial Scale-Up Report, ACSEPT FP7-CP-2007-211 267, 2009.
5 Facility, N. http://fusionwiki.ciemat.es/wiki/LNF:Technology#NAYADE_Co60_irradiation_facility (accessed October 2020)..
6 R.A. Leonard, Design principles and applications of centrifugal contactors for solvent extraction, in: Ion Exchange and Solvent Extraction, CRC Press, 2009, pp. 576-629.
7 D. Magnusson, B. Christiansen, R. Malmbeck, J.P. Glatz, Investigation of the radiolytic stability of a CyMe4-BTBP based SANEX solvent, Radiochim. Acta 97 (9) (2009) 497-502.
8 I. Sanchez-Garcia, L.J. Bonales, H. Galan, J.M. Perlado, J. Cobos, Radiolytic Degradation of sulfonated BTP and acetohydroxamic acid under EURO-GANEX conditions, Radiat. Phys. Chem. 183 (2021), 109402.   DOI
9 D.R. Peterman, L.G. Olson, Summary of ALSEP Test Loop Solvent Irradiation Testing, Idaho National Laboratory.(INL), 2016.
10 D. Peterman, A. Geist, B. Mincher, G. Modolo, M.H. Galan, L. Olson, R. McDowell, Performance of an i-SANEX system based on a water-soluble BTP under continuous irradiation in a γ-radiolysis test loop, Ind. Eng. Chem. Res. 55 (39) (2016) 10427-10435.   DOI
11 R. Taylor, M. Carrott, H. Galan, A. Geist, X. Heres, C. Maher, C. Mason, R. Malmbeck, M. Miguirditchian, G. Modolo, The EURO-GANEX process: current status of flowsheet development and process safety studies, Procedia Chem. 21 (2016) 524-529.   DOI
12 M. Carrott, K. Bell, J. Brown, A. Geist, C. Gregson, X. Heres, C. Maher, R. Malmbeck, C. Mason, G. Modolo, Development of a new flowsheet for coseparating the transuranic actinides: the "EURO-GANEX" process, Solvent Extr. Ion Exch. 32 (5) (2014) 447-467.   DOI
13 D.R. Peterman, B.J. Mincher, C.L. Riddle, R.D. Tillotson, Summary Report on Gamma Radiolysis of TBP/n-dodecane in the Presence of Nitric Acid Using the Radiolysis/hydrolysis Test Loop, Idaho National Laboratory (INL), 2010.
14 B.J. Mincher, G. Modolo, S.P. Mezyk, The effects of radiation chemistry on solvent extraction 3: a review of actinide and lanthanide extraction, Solvent Extr. Ion Exch. 27 (5-6) (2009) 579-606.   DOI
15 B.J. Mincher, G. Modolo, S.P. Mezyk, The effects of radiation chemistry on solvent extraction 4: separation of the trivalent actinides and considerations for radiation-resistant solvent systems, Solvent Extr. Ion Exch. 28 (4) (2010) 415-436.   DOI
16 M.C. Charbonnel, L. Berthon, B. Cames, L. Venault, S. Peuget, In Overview of the French Radiation Chemistry Studies, Radical Behavior Workshop, 2015. Idaho, July 20-22; Idaho.
17 Y. Sasaki, Y. Sugo, S. Suzuki, S. Tachimori, The novel extractants, diglycolamides, for the extraction of lanthanides and actinides in HNO3-n-dodecane system, Solvent Extr. Ion Exch. 19 (1) (2001) 91-103.   DOI
18 R. Malmbeck, D. Magnusson, S. Bourg, M. Carrott, A. Geist, X. Heres, M. Miguirditchian, G. Modolo, U. Mullich, C. Sorel, Homogenous recycling of transuranium elements from irradiated fast reactor fuel by the EURO-GANEX solvent extraction process, Radiochim. Acta 107 (9-11) (2019) 917-929.   DOI
19 I. Sanchez-Garcia, H. Galan, J.M. Perlado, J. Cobos, Stability studies of GANEX system under different irradiation conditions, EPJ Nucl. Sci. Technol. 5 (2019) 19.   DOI
20 J.-M. Adnet, M. Miguirditchian, C. Hill, X. Heres, M. Lecomte, M. Masson, P. Brossard, P. Baron, In Development of new hydrometallurgical processes for actinide recovery: GANEX concept, Proceedings of Global, Paper no 119 (2005).
21 Y. Sugo, Y. Sasaki, S. Tachimori, Studies on hydrolysis and radiolysis of N, N, N', N'-tetraoctyl-3-oxapentane-1, 5-diamide, Radiochim. Acta 90 (3) (2002) 161-165.   DOI
22 L. Berthon, J. Morel, N. Zorz, C. Nicol, H. Virelizier, C. Madic, DIAMEX process for minor actinide partitioning: hydrolytic and radiolytic degradations of malonamide extractants, Separ. Sci. Technol. 36 (5-6) (2001) 709-728.   DOI
23 P. Baron, S. Cornet, E. Collins, G. DeAngelis, G. Del Cul, Y. Fedorov, J. Glatz, V. Ignatiev, T. Inoue, A. Khaperskaya, A review of separation processes proposed for advanced fuel cycles based on technology readiness level assessments, Prog. Nucl. Energy 117 (2019), 103091.   DOI
24 Nunez, A.; Galan, H.; Cobos, J., TODGA degradation compounds: properties and effects on extraction systems-5400. In GLOBAL 2015 Proceedings..
25 E. Collins, G. DelCul, B. Spencer, R. Jubin, C. Maher, I.-T. Kim, H. Lee, Y.S. Federov, V. Saprykin, V. Beznosyuk, State-of-the-art Report on the Progress of Nuclear Fuel Cycle Chemistry, Organisation for Economic Co-Operation and Development, 2018.
26 International Atomic Energy Agency, Spent Fuel Reprocessing Options, IAEA-TECDOC-CD-1587, IAEA, Vienna, 2009.
27 M. Sypula, A. Wilden, C. Schreinemachers, R. Malmbeck, A. Geist, R. Taylor, G. Modolo, Use of polyaminocarboxylic acids as hydrophilic masking agents for fission products in actinide partitioning processes, Solvent Extr. Ion Exch. 30 (7) (2012) 748-764.   DOI
28 A. Geist, U. Mullich, D. Magnusson, P. Kaden, G. Modolo, A. Wilden, T. Zevaco, 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, Solvent Extr. Ion Exch. 30 (5) (2012) 433-444.   DOI
29 R. Taylor, I. May, A. Wallwork, I. Denniss, N. Hill, B.Y. Galkin, B.Y. Zilberman, Y.S. Fedorov, The applications of formo-and aceto-hydroxamic acids in nuclear fuel reprocessing, J. Alloys Compd. 271 (1998) 534-537.
30 M. Carrott, C. Gregson, R. Taylor, Neptunium extraction and stability in the GANEX solvent: 0.2 M TODGA/0.5 M DMDOHEMA/kerosene, Solvent Extr. Ion Exch. 31 (5) (2013) 463-482.   DOI
31 M. Carrott, A. Geist, X. Heres, S. Lange, R. Malmbeck, M. Miguirditchian, G. Modolo, A. Wilden, R. Taylor, 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, Hydrometallurgy 152 (2015) 139-148.   DOI
32 G.P. Horne, S.P. Mezyk, N. Moulton, J.R. Peller, A. Geist, Time-resolved and steady-state irradiation of hydrophilic sulfonated bis-triazinyl-(bi) pyridines-modelling radiolytic degradation, Dalton Trans. 48 (14) (2019) 4547-4554.   DOI
33 P. Joly, E. Boo, ROADMAP-actinide Separation Processes, Euratom Research and Training Programme on Nuclear Energy, 2015.
34 M. Miguirditchian, C. Sorel, B. Cames, I. Bisel, P. Baron, D. Espinoux, J. Calor, C. Viallesoubranne, B. Lorrain, M. Masson, In HA demonstration in the Atalante facility of the GANEX 1st cycle for the selective extraction of Uranium from HLW, Proc. GLOBAL (2009) 1032-1035.
35 C.A. Zarzana, G.S. Groenewold, B.J. Mincher, S.P. Mezyk, A. Wilden, H. Schmidt, G. Modolo, J.F. Wishart, A.R. Cook, A comparison of the γ-radiolysis of TODGA and T (EH) DGA using UHPLC-ESI-MS analysis, Solvent Extr. Ion Exch. 33 (5) (2015) 431-447.   DOI
36 G. Modolo, H. Asp, C. Schreinemachers, H. Vijgen, Development of a TODGA based process for partitioning of actinides from a PUREX raffinate Part I: batch extraction optimization studies and stability tests, Solvent Extr. Ion Exch. 25 (6) (2007) 703-721.   DOI
37 M. Salvatores, Nuclear fuel cycle strategies including partitioning and transmutation, Nucl. Eng. Des. 235 (7) (2005) 805-816.   DOI
38 C. Poinssot, C. Rostaing, S. Greandjean, B. Boullis, Recycling the actinides, the cornerstone of any sustainable nuclear fuel cycles, Procedia Chem. 7 (2012) 349-357.   DOI
39 S. Bourg, A. Geist, J.M. Adnet, C. Rhodes, B.C. Hanson, Partitioning and transmutation strategy R&D for nuclear spent fuel: the SACSESS and GENIORS projects, EPJ Nucl. Sci. Technol. 6 (2020) 35.   DOI
40 A. Geist, J.M. Adnet, S. Bourg, C. Ekberg, H. Galan, P. Guilbaud, M. Miguirditchian, G. Modolo, C. Rhodes, R. Taylor, An overview of solvent extraction processes developed in Europe for advanced nuclear fuel recycling, part 1-heterogeneous recycling, Separ. Sci. Technol. (2020) 1-16.
41 Y. Sugo, Y. Izumi, Y. Yoshida, S. Nishijima, Y. Sasaki, T. Kimura, T. Sekine, H. Kudo, Influence of diluent on radiolysis of amides in organic solution, Radiat. Phys. Chem. 76 (5) (2007) 794-800.   DOI
42 L. Berthon, S. Journet, V. Lalia, J. Morel, N. Zorz, C. Berthon, B. Amekraz, Use of Chromatographic Techniques to Study a Degraded Solvent for Minor Actinides Partitioning: Qualitative and Quantitative Analysis, CEA VALRHO, 2004.
43 S.A. Ansari, P.N. Pathak, V.K. Manchanda, M. Husain, A.K. Prasad, V.S. Parmar, N,N,N',N'-Tetraoctyl Diglycolamide (TODGA): a promising extractant for actinide-partitioning from high-level waste (HLW), Solvent Extr. Ion Exch. 23 (4) (2005) 463-479.   DOI
44 I. Sanchez-Garcia, H. Galan, J.M. Perlado, J. Cobos, Development of experimental irradiation strategies to evaluate the robustness of TODGA and water-soluble BTP extraction systems for advanced nuclear fuel recycling, Radiat. Phys. Chem. 177 (2020), 109094.   DOI
45 M. Carrott, O. Fox, C. Maher, C. Mason, R.J. Taylor, S.I. Sinkov, G.R. Choppin, Solvent extraction behavior of plutonium (IV) ions in the presence of simple hydroxamic acids, Solvent Extr. Ion Exch. 25 (6) (2007) 723-745.   DOI
46 H. Galan, A. Nunez, A.G. Espartero, R. Sedano, A. Durana, J. de Mendoza, Radiolytic stability of TODGA: characterization of degraded samples under different experimental conditions, Procedia Chem. 7 (2012) 195-201.   DOI
47 B.J. Mincher, G. Modolo, S.P. Mezyk, The effects of radiation chemistry on solvent extraction: 1. Conditions in acidic solution and a review of TBP radiolysis, Solvent Extr. Ion Exch. 27 (1) (2009) 1-25.   DOI
48 INTERNATIONAL ATOMIC ENERGY AGENCY, Assessment of Partitioning Processes for Transmutation of Actinides, 2010. Vienna.