Monitoring the plutonium depletion in dissolution residues of a spent fuel solution using a surrogate and plutonium isot
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Monitoring the plutonium depletion in dissolution residues of a spent fuel solution using a surrogate and plutonium isotope ratio measurements Alexandre Quemet1 · Emilie Buravand1 · Brigitte Catanese1 · Patrick Huot1 · Vincent Dalier1 · Alexandre Ruas2 Received: 30 March 2020 © Akadémiai Kiadó, Budapest, Hungary 2020
Abstract This study presents the development of an innovative experiment using a surrogate, for monitoring the depletion kinetics of plutonium dissolution residues in an irradiated fuel dissolution solution containing a high plutonium concentration. The surrogate, a (U,Pu)O2 compound, was synthesized from a plutonium having an isotopic composition different from the dissolution solution. This helps monitoring the plutonium residue depletion by TIMS measurements of the 240Pu/239Pu isotope ratio. Repeatability better than 83 ppm was achieved for the 240Pu/239Pu ratios in each aliquot of the dissolution profiles allowing qualitative and quantitative interpretation of the kinetic evolution that could not be reached by a conventional direct concentration determination. Keywords Dissolution · Residues · Plutonium · TIMS · Isotope ratio · Depletion kinetics
Introduction Along with uranium, plutonium is an essential element in the nuclear fuel cycle [1–4]. Plutonium is present in the reprocessed fuel, the Mixed OXide fuel (MOX) at 5–10% in weight for use in pressurized water reactor and at 20–30% in weight for use in fast-neutron reactor [5, 6]. MOX plutonium amount determination is important to verify the fuel pellet conformity, for nuclear accountancy, for waste management and to manage criticality issues. During the dissolution step of the reprocessing, part of the fuel is not dissolved. The remaining solid particles, called dissolution fines or dissolution residues, include refractory metallic inclusions (mainly composed of platinum group metals), structural component fragments, newly formed phases as zirconium-molybdenum precipitate or insoluble mixed oxide, mainly when MOX fuel are reprocessed [5]. * Alexandre Quemet [email protected] 1
CEA, DES, DMRC, Univ Montpellier, Marcoule, France
Onsite Laboratory Team, Nuclear Material Laboratory, Office of Safeguards Analytical Services, Department of Safeguards, International Atomic Energy Agency, Tokyo Regional Office, Seibunkan Bldg, 9F, 1‑5‑9 Iidabashi, Chiyoda‑ku, Tokyo 102‑0072, Japan
2
The plutonium contained in the residue represents about 0.1% of plutonium initially contained in the MOX fuel but with the Pu-enriched MOX fuels, this value can be higher [5]. The Pu-enriched residue accumulation in dissolvers can be problematic for criticality issues. The ATALANTE facility of the French Alternative Energies and Atomic Energy Commission is dedicated to research on spent nuclear fuel reprocessing. Many studies were performed to better understand MOX fuels: manufacturing, dissolution, recycling,… Among the different MOX fuel R&D topics, one is dedicated to study the Pu residue depletion for criticality issues. An experiment was set up in
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