Abstract
A 1D reactive transport model has been implemented in iCP (interface COMSOL Multiphysics and PhreeqC) to assess the corrosion of Spent Fuel (SF), considered as homogeneous UO2(am,hyd) doped with Pd. The model couples: i) generation of water radiolysis species by alpha and beta radiation considering the complete water radiolysis system with the kinetic reactions involving: H+, OH-, O2, H2O2, H2, HO2-, HO2•, O•, O-, O2-, H•, •OH and e- ii) processes occurring in the spent fuel surface: oxidative dissolution reactions of UO2(am,hyd) and subsequent reduction of oxidized fuel, considering H2 activation by Pd, and iii) corrosion of Fe(s) in oxic and anoxic conditions. Process i) has been implemented in COMSOL and processes ii) and iii) have been implemented in PHREEQC with their kinetic constants being calibrated with different sets of experimental data published in the open literature. The model yields a UO2(am,hyd) dissolution rates similar to the values selected in safety assessments.
Similar content being viewed by others
References
Wu, L., Beauregard, Y., Qin, Z., Rohani, S., Shoesmith, D. W. (2012). A model for the influence of steel corrosion products on nuclear fuel corrosion under permanent disposal conditions. Corrosion Science, 61, 83–91.
Wu, L., Liu, N., Qin, Z., Shoesmith, D.W. (2014a). Modeling the radiolytic corrosion of fractured nuclear fuel under permanent disposal conditions. Journal of The Electrochemical Society, 161(8), E3259–E3266.
Wu, L., Qin, Z., Shoesmith, D. W. (2014b). An improved model for the corrosion of used nuclear fuel inside a failed waste container under permanent disposal conditions. Corrosion Science, 84, 85–95.
Jerden, J. L., Frey, K., Ebert, W. (2015). A multiphase interfacial model for the dissolution of spent nuclear fuel. Journal of Nuclear Materials, 462, 135–146.
Odorowski, M., (2015). Etude de l’altération de la matrice (U,Pu)O2 du combustible irradié en conditions de stockage géologique: Approche expérimentale et modélisation géochimique. Doctoral Thesis.
Nardi, A., Idiart, A., Trinchero, P., de Vries, L. M., and J. Molinero (2014). Interface COMSOL-PHREEQC (iCP), an efficient numerical framework for the solution of coupled multiphysics and geochemistry. Computers & Geosciences 69: 10–21.
COMSOL Multiphysics, https://www.comsol.com/
Parkhurst, D. L., and C. A. J. Appelo (2013) Description of input and examples for PHREEQC version 3—A computer program for speciation, batch-reaction, one-dimensional transport, and inverse geochemical calculations, U.S. Geological Survey Techniques and Methods, book 6, chap. A43, 497 p.
Tian, Z., Jiang, S. B., Jia, X. (2017). Accelerated Monte Carlo simulation on the chemical stage in water radiolysis using GPU. Physics in Medicine & Biology, 62(8), 3081.
Cera, E., Bruno, J., Duro, L., Eriksen, T. (2006). Experimental determination and chemical modelling of radiolytic processes at the spent fuel/wáter interface. SKB TR 06-07, Svensk Kärnbränslehantering AB.
Kelm, M., Bohnert, E. (2004) A kinetic model for the radiolysis of chloride brine, its sensitivity against model parameters and a comparison with experiments, Forschungszentreum Karlsruhe, FZKA 6977.
Eriksen, T. E., Jonsson, M., Merino, J. (2008). Modelling of time resolved and long contact time dissolution studies of spent nuclear fuel in 10 mM carbonate solution–a comparison between two different models and experimental data. Journal of Nuclear Materials, 375(3), 331–339
Merino, J., Cera, E., Bruno, J., Quinones, J., Casas, I., Clarens, F., … & Martínez-Esparza, A. (2005). Radiolytic modelling of spent fuel oxidative dissolution mechanism. Calibration against UO2 dynamic leaching experiments. Journal of nuclear materials, 346(1), 40–47.
Trummer, M., Nilsson, S., Jonsson, M. (2008). On the effects of fission product noble metal inclusions on the kinetics of radiation induced dissolution of spent nuclear fuel. Journal of Nuclear Materials, 378(1), 55–59.
ThermoChimie Database version 9b0. Andra thermodynamic database for performance assessment https://www.thermochimie-tdb.com/pages/version.php
Bruno, J., Casas, I., Puigdomènech, I. (1991). The kinetics of dissolution of UO2 under reducing conditions and the influence of an oxidized surface layer (UO2+x): Application of a continuous flow-through reactor. Geochimica et Cosmochimica Acta, 55(3), 647–658.
Zetterström Evins, L., Juhola, P., Vähänen, M. (Eds.) (2014). REDUPP Final Report. POSIVA report 2014-12.1. 128 pp. http://www.posiva.fi/files/3672/WR2014-12.1.pdf
Bruno, J., Merino, J., Tamayo, A., Ferry, C., Quiñones, J., Iglesias, E., Rodriguez Villagra, N., Nieto, J.M., Martínez-Esparza, A., Loida, A., Metz, V., Jonsson, M., Ekeroth, E. and Grambow, B. (2005) MICADO project EURATOM specific programme for research and training on nuclear energy, FINAL D3.1 Deliverable: Application of models to selected datasets, NUWASTE-2005/6-3.2.1.1-2
Féron, D., Crusset, D., Gras, J. M. (2008). Corrosion issues in nuclear waste disposal. Journal of Nuclear Materials, 379(1–3), 16–23.
Andra Dossier 2005 Argile: Évaluation de la faisabilité du stockage géologique en formation argileuse. Document de synthèse. Andra, Paris.
Martínez Esparza, A., Cuñado, M. A., Gago, J. A., Quiñones, J., Iglesias, E., Cobos, J., González de la Huebra, A., Cera, E., Merino, J., Bruno, J., de Pablo, J., Casas, I., Clarens, F., Giménez, J. (2005). Development of a Matrix Alteration Model (MAM), ENRESA PT-01-2005
Svensk Kärnbränslehantering AB (2010). Data report for safety assessment SR-Site. SKB TR-10-52.
POSIVA (2013). Safety Case for the Disposal of Spent Nuclear Fuel at Olkiluoto - Models and Data for the Repository System 2012. POSIVA 2013-01
Johnson, L., (2014). A model for radionuclide release from spent UO2 and MOX fuel. NAB 13-37
NWMO (2015). Technical Program for Long-Term Management of Canada’s Used Nuclear Fuel–Annual Report 2014. NWMO TR-2015-01
AEA (2015). Preliminary Assessment of Geological Disposal System for Spent Fuel in Japan - First Progress Report on Direct Disposal. JAEA-Research, 2015–016.
Author information
Authors and Affiliations
Rights and permissions
About this article
Cite this article
Riba, O., Coene, E., Silva, O. et al. Spent fuel alteration model integrating processes of different time-scales. MRS Advances 5, 159–166 (2020). https://doi.org/10.1557/adv.2020.51
Published:
Issue Date:
DOI: https://doi.org/10.1557/adv.2020.51