journal article·2023-08Open access

Beyond U/Pu separation: Separation of americium from the highly active PUREX raffinate

P. Zsabka, A. Wilden, K. Van Hecke, G. Modolo, M. Verwerft, T. Cardinaels

Abstract

This review provides a comprehensive overview of published hydrometallurgical chemical processes capable of separating americium from curium and the lanthanides. A search for highly selective and robust americium separation methods is motivated by the fact that americium isotopes contribute significantly to the long-term heat load and residual radiotoxicity of high level waste originating from the PUREX process, nowadays still the key reprocessing technology to recycle uranium and plutonium from spent nuclear fuel. The separation (partitioning) and subsequent nuclear transmutation (or burning) of americium would allow a substantial improvement in the construction of an underground final repository and provide safety benefits – highly relevant for the exploitation of such a facility over extended periods of time. Besides the discussion of basic properties of the various separation methods, an evaluation of their compatibility with upstream and downstream processes as well as the treatment of secondary waste streams is also provided.
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Research context

OpenAlex topics: Radioactive element chemistry and processing · Nuclear materials and radiation effects · Chemical Synthesis and Characterization

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References (100+)

Show source-provided references
1. Boundary conditions for separation and conditioning, Report, E. Weetjens, J. Govaerts, J. Perko, K. Van Hecke, K. Govers, SCK CEN, 2019, pp. 1–52., Report No.: SCK CEN/33517036.
2. 2022 · 1
3. RED-IMPACT Impact of Partitioning, Transmutation and Waste Reduction Technologies on the Final Nuclear Waste Disposal, Report, D. Greneche, B. Quiniou, L. Boucher, M. Delpech, E. Gonzalez, F. Alvarez, M.A. Cuñado, G. Serrano, J.L. Cormenzana, W. Kuckshinrichs, R. Odoj, W. von Lensa, J. Wallenius, D. Westlén, C. Zimmermann, J. Marivoet, in Schriften des Forschungszentrums Jülich Reihe Energie & Umwelt /Energy & Environment, Vol. 15 (Eds.: W. von Lensa, R. Nabbi, M. Rossbach), Forschungszentrum Jülich GmbH Institut für Energieforschung (IEF) Sicherheitsforschung und Reaktortechnik (IEF-6), Jülich, Germany, 2008.
4. Impact of partitioning and transmutation on LWR high-level waste disposal10.1080/18811248.2008.9711418 ↗
5. Thermal impact on geological disposal of hull and end piece wastes resulting from high-burn-up operation of LWR and introduction of MOX fuels into LWR10.1080/18811248.2007.9711551 ↗
6. A report by the working party on scientific issues of reactor systems - organisation for economic co-operation and development, report
7. Plutonium and minor actinides incineration options using innovative Na-cooled fast reactors: impacting on phasing-out and on-going fuel cycles10.1016/j.pnucene.2014.07.034 ↗
8. 2020
9. 2021
10. Assessment of the anticipated environmental footprint of future nuclear energy systems. evidence of the beneficial effect of extensive recycling10.3390/en10091445 ↗
11. A review of environmental and economic implications of closing the nuclear fuel cycle—part one: wastes and environmental impacts10.3390/en15041433 ↗
12. A review of environmental and economic implications of closing the nuclear fuel cycle—part two: economic impacts10.3390/en15072472 ↗
13. Separation and recovery of Cm from Cm–Pu mixed oxide samples containing Am impurity10.1007/s10967-012-2304-y ↗
14. An overview of solvent extraction processes developed in Europe for advanced nuclear fuel recycling, part 1 — Heterogeneous recycling10.1080/01496395.2020.1795680 ↗
15. Aspects of fabrication of curium-based fuels and targets10.1016/S0022-3115(03)00168-5 ↗
16. Aqueous partitioning of minor actinides by different processes10.1080/15422119.2010.545466 ↗
17. Madic · 2007
18. A review of the demonstration of innovative solvent extraction processes for the recovery of trivalent minor actinides from PUREX raffinate10.1524/ract.2012.1962 ↗
19. The SACSESS hydrometallurgy domain — an overview10.1016/j.proche.2016.10.031 ↗
20. An overview of solvent extraction processes developed in Europe for advanced nuclear fuel recycling, Part 2 — Homogeneous recycling10.1080/01496395.2021.2001531 ↗
21. 2018
22. Use of soft heterocyclic N-donor ligands to separate actinides and lanthanides10.1021/ic3008848 ↗
23. Recent trends in the search for new extractants10.1080/08827500008914166 ↗
24. Complexation and extraction of trivalent actinides and lanthanides by triazinylpyridine N-donor ligands10.1021/cr3003399 ↗
25. Recent progress in trivalent actinide and lanthanide solvent extraction and coordination chemistry with triazinylpyridine N donor ligands10.1080/07366299.2020.1831235 ↗
26. Solvent extraction systems for mutual separation of Am(III) and Cm(III) from nitric acid solutions. A review of recent state-of-the-art10.1080/07366299.2020.1856998 ↗
27. A review of separation processes proposed for advanced fuel cycles based on technology readiness level assessments10.1016/j.pnucene.2019.103091 ↗
28. The European pyrometallurgical processing research program PYROREP: main issues, Global 2003
29. 2021 · 1
30. An introduction to some aspects of solvent extraction chemistry in hydrometallurgy10.1016/0304-386X(82)90014-7 ↗
31. Hard and soft acids and bases10.1021/ja00905a001 ↗
32. Kolarik · 1991 · 1
33. Selective extraction of Am(III) over Eu(III) by 2,6-ditriazolyl- and 2,6-ditriazinylpyridines10.1080/07360299908934598 ↗
34. New partitioning techniques for minor actinides. Final Report, NEWPART, C. Madic, M.J. Hudson, J.O. Liljenzin, J.P. Glatz, R. Nannicini, A. Facchini, Z. Kolarik, R. Odoj, European Commission Brussels, 2000, Project report EUR 19149.
35. Partnew - New solvent extraction processes for minor actinides - final report, C. Madic, F. Testard, M.J. Hudson, J.O. Liljenzin, B. Christiansen, M. Ferrando, A. Facchini, A. Geist, G. Modolo, A. Gonzalez-Espartero, J.d. Mendoza, France, 2004, Report No.: CEA-R-6066.
36. Lewis · 2009
37. Comparative solution chemistry of the 4f and 5f elements10.1016/0925-8388(94)09002-5 ↗
38. Hudson · 2013 · 9 · 177
39. Quantum chemical studies of selective back-extraction of Am(III) from Eu(III) and Cm(III) with two hydrophilic 1,10-phenanthroline-2,9-bis-triazolyl ligands10.1515/ract-2019-3197 ↗
40. Method for separating trivalent americium from trivalent curium
41. Demonstration of the LUCA process for the separation of americium(III) from curium(III), californium(III), and lanthanides(III) in acidic solution using a synergistic mixture of bis(chlorophenyl)dithiophosphinic acid and tris(2-ethylhexyl)phosphate10.1524/ract.2010.1708 ↗
42. Separation of americium by liquid-liquid extraction using diglycolamides water-soluble complexing agents10.1016/j.proche.2016.10.019 ↗
43. New insight into the americium/curium separation by solvent extraction using diglycolamides10.1080/07366299.2014.1000792 ↗
44. Complexation of Ln(III) and Am(III) with the Hydrosoluble TEDGA: speciation and thermodynamics studies10.1016/j.proche.2012.10.005 ↗
45. Implementation of americium separation from a PUREX raffinate10.1016/j.proche.2012.10.030 ↗
46. Consolidation of the EXAm process: towards the reprocessing of a concentrated PUREX raffinate10.1016/j.proche.2016.10.027 ↗
47. Americium recovery from highly active PUREX raffinate by solvent extraction: the EXAm process. a review of 10 years of R&D10.1080/07366299.2020.1753922 ↗
48. Baron · 2003
49. Complexation of actinide(III) and lanthanide(III) with HTPAEN for a separation of americium from curium and lanthanides10.1021/acs.inorgchem.7b00603 ↗
50. Modeling and flowsheet design of an am separation process using TODGA and H4TPAEN10.1016/j.proche.2016.10.032 ↗
51. Separation of Am (III) by solvent extraction using water-soluble H4tpaen derivatives10.1016/j.tet.2015.06.015 ↗
52. Direct selective extraction of trivalent americium from PUREX raffinate using a combination of CyMe4BTPhen and TEDGA—a feasibility study10.1080/07366299.2017.1326761 ↗
53. Selective extraction of Am(III) from PUREX raffinate: the AmSel system10.1080/07366299.2015.1129192 ↗
54. Complexation and extraction studies of trivalent actinides and lanthanides with water-soluble and CHON-compatible ligands for the selective extraction of americium10.1021/acs.inorgchem.2c02871 ↗
55. Aqueous complexes for efficient size-based separation of americium from curium10.1021/ic500244p ↗
56. Solvent extraction separation of trivalent americium from curium and the lanthanides10.1080/07366299.2015.1046292 ↗
57. Novel extractant, NTAamide, and its combination with TEDGA for mutual separation of Am/Cm/Ln10.1080/07366299.2013.836422 ↗
58. Highly practical and simple ligand for separation of Am(III) and Eu(III) from highly acidic media10.2116/analsci.32.477 ↗
59. High-performance alkyl diamide amine and water-soluble diamide ligand for separating of Am(III) from Cm(III)10.2116/analsci.33.239 ↗
60. Continuous extraction and separation of Am(III) and Cm(III) using a highly practical diamide amine extractant10.1080/00223131.2017.1299050 ↗
61. Thermodynamic study on the synergistic mixture of Bis(chlorophenyl)dithiophosphinic acid and tris(2-ethylhexyl)phosphate for separation of actinides(III) from lanthanides(III)10.1081/SEI-200056515 ↗
62. Hydrolysis and radiation stability of the alina solvent for actinide(III)/lanthanide(III) separation during the partitioning of minor actinides10.1081/SEI-120003021 ↗
63. X. Heres, P. Baron, Increase in the separation factor between americium and curium and/or between lanthanides in a liquid-liquid extraction process, Patent WO/2011/012579, 2011.
64. Numerical code in the service of La Hague plant operations10.1016/j.proche.2016.10.017 ↗
65. Solvent extraction separation of trivalent americium from curium and the lanthanides10.1080/07366299.2015.1046292 ↗
66. Actinide-lanthanide separation process-ALSEP10.1021/ie403569e ↗
67. Closing the nuclear fuel cycle with a simplified minor actinide lanthanide separation process (ALSEP) and additive manufacturing,10.1038/s41598-019-48619-x ↗
68. Countercurrent actinide lanthanide separation process (ALSEP) demonstration test with a simulated PUREX raffinate in centrifugal contactors on the laboratory scale10.3390/app10207217 ↗
69. Extraction behavior of metal ions by TODGA, DOODA, MIDOA, and NTAamide extractants from HNO3ton-dodecane10.1080/07366299.2013.800431 ↗
70. Highly efficient separation of actinides from lanthanides by a phenanthroline-derived bis-triazine ligand10.1021/ja203378m ↗
71. Radiation influencing of the extraction properties of the CyMe4-BTBP and CyMe4-BTPhen solvents with FS-1310.1016/j.proche.2016.10.025 ↗
72. Fluorinated carbonates as new diluents for extraction and separation of f-block elements10.1080/07366299.2019.1708004 ↗
73. Gamma radiolysis of TODGA and CyMe4BTPhen in the ionic liquid tri-n-octylmethylammonium nitrate10.1080/07366299.2019.1710918 ↗
74. Selective extraction of americium from curium and the lanthanides by the lipophilic ligand CyMe4BTPhen dissolved in aliquat-336 nitrate ionic liquid10.1080/07366299.2019.1708006 ↗
75. Separation of the minor actinides americium(III) and curium(III) by hydrophobic and hydrophilic BTPhen ligands: exploiting differences in their rates of extraction and effective separations at equilibrium10.1080/07366299.2018.1429358 ↗
76. Modelling of the Am(III) – Cm(III) kinetic separation effect observed during metal ion extraction by bis-(1,2,4)-triazine ligands10.1080/01496395.2017.1384017 ↗
77. Selective extraction of trivalent actinides using CyMe4BTPhen in the ionic liquid aliquat-336 nitrate10.1039/D0RA10445K ↗
78. The EURATOM FP7 project on actinide separation from spent nuclear fuels10.1515/nuka-2015-0152 ↗
79. Development of a selective americium separation process using H4TPAEN as water-soluble stripping agent10.1080/07366299.2019.1643569 ↗
80. Water soluble PDCA derivatives for selective Ln(III)/An(III) and Am(III)/Cm(III) separation10.1080/07366299.2014.974449 ↗
81. An efficient design for the rigid assembly of four bidentate chromophores in water-stable highly luminescent lanthanide complexes10.1002/anie.200502231 ↗
82. Solvent extraction and fluorescence spectroscopic investigation of the selective Am(III) complexation with TS-BTPhen10.1080/07366299.2016.1151308 ↗
83. TS-BTPhen as a promising hydrophilic complexing agent for selective Am(III) separation by solvent extraction10.1515/nuka-2015-0120 ↗
84. Kaufholz · 2017
85. Hydrophilic sulfonated bis-1,2,4-triazine ligands are highly effective reagents for separating actinides(III) from lanthanides(III) via selective formation of aqueous actinide complexes10.1039/C5SC01328C ↗
86. Optimization and single-stage centrifugal contactor experiments with the novel hydrophilic complexant PyTri-Diol for the i-SANEX process10.1080/07366299.2018.1507134 ↗
87. Hydrophilic clicked 2,6-bis-triazolyl-pyridines endowed with high actinide selectivity and radiochemical stability: toward a closed nuclear fuel cycle10.1021/jacs.6b03106 ↗
88. Hydrophilic 2,9-bis-triazolyl-1,10-phenanthroline ligands enable selective Am(III) separation: a step further towards sustainable nuclear energy10.1039/C7CC01855J ↗
89. Solvent extraction studies for the separation of trivalent actinides from lanthanides with a triazole-functionalized 1,10-phenanthroline extractant10.1080/07366299.2020.1790105 ↗
90. Higher oxidation states of americium: preparation, characterization and use for separations10.1021/cr100181f ↗
91. Development of the SESAME process, Conference proceedings
92. S. Picart, D. Chartier, L. Donnet, J.M Adnet, Electrochemical oxidation of americium in nitric medium: study of reaction mechanisms, Report, CEA Saclay, Direction du Cycle du Combustible, 91 - Gif-sur-Yvette (France), 383 (2000) 192–197, Report No.: R–5892.
93. 1992-2017: 25 years of success story on minor actinides partitioning processes development, conference paper
94. Separation of long-lived radionuclides from high active nuclear waste10.1016/S1631-0705(02)01370-1 ↗
95. The chemistry of americium. I. a study of the preparation of Am (V) and its behavior by means of TTA extraction10.1246/bcsj.43.89 ↗
96. The chemistry of americium. II. The behavior of Am(III), Am(V), and Am(VI) in column chromatography, with Bis(2-ethylhexyl)phosphoric acid used as the extractant10.1246/bcsj.47.635 ↗
97. Analytical oxidation of americium with sodium perxenate10.1021/ac60222a002 ↗
98. A TRUEX-based separation of americium from the lanthanides10.1080/07366299.2011.539146 ↗
99. Extraction of americium(VI) by a neutral phosphonate ligand10.1007/s10967-009-0153-0 ↗
100. Tributylphosphate extraction behavior of bismuthate-oxidized americium10.1021/ic800667h ↗