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Modeling and Flowsheet Design of an Am Separation Process Using TODGA and H₄TPAEN

Vanel, V.; Marie, C.; Kaufholz, P.; Montuir, M.; Boubals, N.; Wilden, A.; Modolo, G.; Geist, A.; Sorel, C.

Abstract (englisch):
Recycling americium from spent fuels is an important consideration for the future nuclear fuel cycle, as americium is the main contributor to the long-term radiotoxicity and heat power of the final waste, after separation of uranium and plutonium using the PUREX process. The separation of americium alone from a PUREX raffinate can be achieved by co-extracting lanthanide (Ln(III)) and actinide (An(III)) cations into an organic phase containing the diglycolamide extractant TODGA, and then stripping Am(III) with selectivity towards Cm(III) and lanthanides. The water soluble ligand H4TPAEN was tested to selectively strip Am from a loaded organic phase.

Based on experimental data obtained by Jülich, NNL and CEA laboratories since 2013, a phenomenological model has been developed to simulate the behavior of americium, curium and lanthanides during their extraction by TODGA and their complexation by H4TPAEN (complex stoichiometry, extraction and complexation constants, kinetics). The model was gradually implemented in the PAREX code and helped to narrow down the best operating conditions. Thus, the following modifications of initial operating conditions were proposed:

An increase in the concentration of TPAEN as much as the solubility limit allows.

An improvement of the lanthanide scrubbing from the americium flow by adding nitrates to the aqueous phase.


A qualification of the model was begun by comparing on the one hand constants determined with the model to those measured experimentally, and on the other hand, simulation results and experimental data on new independent batch experiments.

A first sensitivity analysis identified which parameter has the most dominant effect on the process. ... mehr

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Volltext §
DOI: 10.5445/IR/1000062648
Originalveröffentlichung
DOI: 10.1016/j.proche.2016.10.032
Coverbild
Zugehörige Institution(en) am KIT Institut für Nukleare Entsorgung (INE)
Publikationstyp Zeitschriftenaufsatz
Jahr 2016
Sprache Englisch
Identifikator ISSN: 1876-6196
urn:nbn:de:swb:90-626485
KITopen-ID: 1000062648
HGF-Programm 32.01.11 (POF III, LK 01)
Erschienen in Procedia chemistry
Band 21
Seiten 223–230
Bemerkung zur Veröffentlichung ATALANTE 2016 International Conference on Nuclear Chemistry for Sustainable Fuel Cycles
Schlagworte TPAEN; Am separation; extraction and complexation modelling; PAREX code
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