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

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. A flowsheet was proposed for a spiked test in centrifugal contactors performed with a simulated PUREX raffinate with trace amounts of Am and Cm. If the feasibility of the process is confirmed, the results of this test will be used to consolidate the model and to design a flowsheet for a test on a genuine PUREX raffinate. This work is the result of collaborations in the framework of the SACSESS European Project.