Contribution of phases segregated from the UO2 matrix to the release of radionuclides from spent nuclear fuel and duration of the Instant Release Fraction (IRF)

During the dissolution of the spent nuclear fuel (SNF) some radionuclides are released to the solution simultaneously from different sources in the fuel. This is of particular importance to some radionuclides that contribute to the Instant Release Fraction (IRF), which govern the initial radiation d...

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Detalles Bibliográficos
Autores: Espriu Gascon, Alexandra, Martínez Torrents, Albert, Serrano Purroy, Daniel, Giménez Izquierdo, Francisco Javier|||0000-0003-2094-4458, Pablo Ribas, Joan de|||0000-0001-9538-7321, Casas Pons, Ignasi|||0000-0002-5419-1645
Tipo de recurso: artículo
Fecha de publicación:2020
País:España
Institución:Universitat Politècnica de Catalunya (UPC)
Repositorio:UPCommons. Portal del coneixement obert de la UPC
Idioma:inglés
OAI Identifier:oai:upcommons.upc.edu:2117/340826
Acceso en línea:https://hdl.handle.net/2117/340826
https://dx.doi.org/10.1016/j.jnucmat.2020.152066
Access Level:acceso abierto
Palabra clave:Radioactive substances
Radioisotopes
IRF
Spent nuclear fuel
Radionuclide
UO2
Substàncies radioactives
Isòtops radioactius
Àrees temàtiques de la UPC::Enginyeria química
Descripción
Sumario:During the dissolution of the spent nuclear fuel (SNF) some radionuclides are released to the solution simultaneously from different sources in the fuel. This is of particular importance to some radionuclides that contribute to the Instant Release Fraction (IRF), which govern the initial radiation dose during the dissolution of the SNF. In this work a model that is able to discriminate between the different contributions responsible for the total concentration of a radionuclide in solution was developed. The model permits to establish that uranium and radionuclides that dissolved congruently with the UO2 matrix came from two sources as a function of time: oxidized phases on the surface of the SNF including fines and the matrix itself. Other radionuclides such as Ru and Rh were released from metallic precipitates with dissolution rates lower than the matrix dissolution rate. In the case of radionuclides that were expected to contribute to the IRF, this work showed that Cs, Rb and Sr had initial release rates higher than uranium because a fraction of such radionuclides were segregated from the matrix during the irradiation. Actually it was calculated that the fraction of those radionuclides in the grain boundaries in a BWR SNF powder sample from the center part of a pellet (burnup 42 MWd/kgU) was 2.1%, 0.9%, and 0.6% for Cs, Rb, and Sr, respectively. In addition, the model permitted to calculate the duration of their contribution to the IRF, matrix dissolution governed the release of such radionuclides after 137 days, 75 days, and 164 days for Cs, Rb, and Sr, respectively (at these times, the contribution of the release from grain boundaries was lower than the 0.1%).