Skip to main content Accessibility help
×
Home
Hostname: page-component-684899dbb8-gblv7 Total loading time: 0.227 Render date: 2022-05-16T22:17:52.535Z Has data issue: true Feature Flags: { "shouldUseShareProductTool": true, "shouldUseHypothesis": true, "isUnsiloEnabled": true, "useRatesEcommerce": false, "useNewApi": true }

Interpretation of Knudsen Cell Experiments to determine the Instant Release Fraction in Spent Fuel Corrosion Scenarios by using a Mechanistic Approach: the Caesium Case

Published online by Cambridge University Press:  01 July 2014

Daniel Serrano-Purroy
Affiliation:
European Commission, Joint Research Centre, Institute for Transuranium Elements, P.O. Box 2340, D-76125 Karlsruhe, Germany
Laura Aldave de las Heras
Affiliation:
European Commission, Joint Research Centre, Institute for Transuranium Elements, P.O. Box 2340, D-76125 Karlsruhe, Germany
Jean-Paul Glatz
Affiliation:
European Commission, Joint Research Centre, Institute for Transuranium Elements, P.O. Box 2340, D-76125 Karlsruhe, Germany
Ondrej Benes
Affiliation:
European Commission, Joint Research Centre, Institute for Transuranium Elements, P.O. Box 2340, D-76125 Karlsruhe, Germany
Jean Yves Colle
Affiliation:
European Commission, Joint Research Centre, Institute for Transuranium Elements, P.O. Box 2340, D-76125 Karlsruhe, Germany
Rosa Sureda
Affiliation:
CTM Centre Tecnològic, Avda. Bases de Manresa 1, 08240 Barcelona, Spain
Ernesto González-Robles
Affiliation:
CTM Centre Tecnològic, Avda. Bases de Manresa 1, 08240 Barcelona, Spain
Joan de Pablo
Affiliation:
CTM Centre Tecnològic, Avda. Bases de Manresa 1, 08240 Barcelona, Spain
Ignasi Casas
Affiliation:
CTM Centre Tecnològic, Avda. Bases de Manresa 1, 08240 Barcelona, Spain
Marc Barrachin
Affiliation:
Institut de Radioprotection et de Sûreté Nucléaire (IRSN), B.P. 3, F-13115 St Paul lez-Durance, France
Roland Dubourg
Affiliation:
Institut de Radioprotection et de Sûreté Nucléaire (IRSN), B.P. 3, F-13115 St Paul lez-Durance, France
Aurora Martínez-Esparza
Affiliation:
ENRESA, C/Emilio Vargas 7, 28043 Madrid, Spain
Get access

Abstract

The Knudsen Effusion Mass Spectrometer (KEMS) and the mechanistic MFPR (Module for Fission Product Release) code are tools which seem particularly interesting to support studies of the Instant Release Fraction (IRF) of Cs from spent nuclear fuel in a final repository. With KEMS, the thermal release of 137Cs and 136Xe were analysed by annealing up to total vaporization (2500K) of high burn-up (60 GWd/tU) Spent Nuclear Fuel (SNF) samples. Powder samples from the centre of the fuel, without high burn-up structure, were used. To determine the IRF, samples were analysed before and after being submitted to corrosion experiments in bicarbonated aqueous media.

MFPR was applied to determine the localization of Cs and fission gases in the SNF at the end of irradiation; the results are compared and supported by dedicated thermodynamics calculations performed for equilibrium conditions at various temperatures and fuel oxygen potentials by the non-ideal thermodynamic MEPHISTA (Multiphase Equilibria in Fuels via Standard Thermodynamic Analysis) database. A possible mechanism for Cs release during thermal annealing is proposed, taking into account inter-granular release and Cs oxide vaporization, atomic diffusion, ternary oxide phase formation and bubble release.

Differences in KEMS release profiles before and after submitting the samples to aqueous corrosion are attributed to the IRF and to changes in the vaporisation mechanism because of differences in the oxygen potential (pO2). The IRF of Cs estimated from the KEMS spectra, consisting on the part located at the grain boundaries and in inter-granular bubbles, is not significantly different from that corresponding to the experimental results found using classical static leaching experiments.

New experimental campaigns are being designed to confirm our interpretation proposed after this first run.

Type
Articles
Copyright
Copyright © Materials Research Society 2014 

Access options

Get access to the full version of this content by using one of the access options below. (Log in options will check for institutional or personal access. Content may require purchase if you do not have access.)

References

Serrano-Purroy, D., Clarens, F., González-Robles, E., Glatz, J.P., Wegen, D.H., de Pablo, J., Casas, I., Giménez, J., Martínez-Esparza, A.. J. Nucl. Mat. 427 249258 (2012).10.1016/j.jnucmat.2012.04.036CrossRef
Serrano-Purroy, D., Casas, I., González-Robles, E., Glatz, J. P., Wegen, D.H., Clarens, F., Giménez, J., de Pablo, J., Martínez-Esparza, A..J. Nucl. Mat. 427 249258 (2012).10.1016/j.jnucmat.2012.04.036CrossRef
Serrano-Purroy, D., Rondinella, V.V., Wegen, D.H.. Characterisation of Irradiated MOX: Static leaching Report, NF-PRO Deliverable 1.4.10. ITU Technical Report JRC-ITU-TPW-2007/37.
González-Robles, E. Study of Radionuclide Release in commercials UO2 Spent Nuclear Fuels, Doctoral Thesis, Universitat Politécnica de Catalunya, 2011.Google Scholar
Rondinella, V.V. Serrano-Purroy, D.. Hiernaut, J.-P., Wegen, D., Papaioannou, D., Barker, M., “Grain boundary inventory and instant release fractions for SBR MOX”, Proc. International High-Level Radioactive Waste Management Conference, Sept 7–9, 2008, Las Vegas, USA, paper 195780, ANS CD-ROM.Google Scholar
de Pablo, J., Serrano-Purroy, D., Gonzalez-Robles, E., Clarens, F., Martínez-Esparza, A., Wegen, D.H., Casas, I., Christiansen, B., Glatz, J.-P., Giménez, J. in Scientific Basis for Nuclear Waste Management XXXVII, edited by Burakov, B.E. and Aloy, A.S., (Mater. Res. Soc. Symp. Proc. 1193, Warrendale, PA, 2009)pp. 613620..Google Scholar
Serrano-Purroy, D., Casas, I., González-Robles, E., Glatz, J.P., Wegen, D.H., Clarens, F., Giménez, J., de Pablo, J., Martínez-Esparza, A.. J. Nucl. Mat. 434, 451-460 (2013).10.1016/j.jnucmat.2011.03.020CrossRef
Hiernaut, J.P., Ronchi, C.. J. Nuc. Mat. 294, 3944 (2001).10.1016/S0022-3115(01)00469-XCrossRef
Hiernaut, J.P., Colle, J.Y., Pflieger-Cuvelier, R., Jonnet, J., Somers, J., Ronchi, C.. J. Nucl. Mat. 344, 246253 (2005).10.1016/j.jnucmat.2005.04.050CrossRef
Colle, J.Y., Hiernaut, J.P., Papaioannou, D., Ronchi, C., Sasahara, A.. J. Nucl. Mat. 348, 229242(2006).10.1016/j.jnucmat.2005.09.024CrossRef
Hiernaut, J.P., Wiss, T., Papaioannou, D., Konings, R.J.M., Rondinella, V.V..J. Nucl. Mat. 372, 215225 (2008).10.1016/j.jnucmat.2007.03.174CrossRef
Veshchunov, M.S, Ozrin, V.D., Shestak, V.E., Tarasov, V.I., Dubourg, R., Nicaise, G., Nucl. Eng. and Des. 236, 179200 (2006).10.1016/j.nucengdes.2005.08.006CrossRef
Veshchunov, M.S., Dubourg, R., Ozrin, V.D., Shestak, V.E., Tarasov, V.I., J. Nucl. Mat. 362, 327335 (2007).10.1016/j.jnucmat.2007.01.081CrossRef
Colle, J.-Y., Maugeri, E. A., Thiriet, C., Talip, Z., Capone, F., Hiernaut, J.-P., Konings, R. J. M., Wiss, T., Colle, Jean-Yves, Maugeri, Emilio A., Thiriet, Catherine, Talip, Zeynep, Capone, Franco, Hiernaut, Jean-Pol, Konings, Rudy J. M., and Wiss, Thierry, Journal of nuclear science deans technology Accepted for publication
Saunders, N., Miodownik, A.P., CALPHAD calculation of phase diagrams, Elsevier Science Ltd, Oxford (1998)Google Scholar

Save article to Kindle

To save this article to your Kindle, first ensure coreplatform@cambridge.org is added to your Approved Personal Document E-mail List under your Personal Document Settings on the Manage Your Content and Devices page of your Amazon account. Then enter the ‘name’ part of your Kindle email address below. Find out more about saving to your Kindle.

Note you can select to save to either the @free.kindle.com or @kindle.com variations. ‘@free.kindle.com’ emails are free but can only be saved to your device when it is connected to wi-fi. ‘@kindle.com’ emails can be delivered even when you are not connected to wi-fi, but note that service fees apply.

Find out more about the Kindle Personal Document Service.

Interpretation of Knudsen Cell Experiments to determine the Instant Release Fraction in Spent Fuel Corrosion Scenarios by using a Mechanistic Approach: the Caesium Case
Available formats
×

Save article to Dropbox

To save this article to your Dropbox account, please select one or more formats and confirm that you agree to abide by our usage policies. If this is the first time you used this feature, you will be asked to authorise Cambridge Core to connect with your Dropbox account. Find out more about saving content to Dropbox.

Interpretation of Knudsen Cell Experiments to determine the Instant Release Fraction in Spent Fuel Corrosion Scenarios by using a Mechanistic Approach: the Caesium Case
Available formats
×

Save article to Google Drive

To save this article to your Google Drive account, please select one or more formats and confirm that you agree to abide by our usage policies. If this is the first time you used this feature, you will be asked to authorise Cambridge Core to connect with your Google Drive account. Find out more about saving content to Google Drive.

Interpretation of Knudsen Cell Experiments to determine the Instant Release Fraction in Spent Fuel Corrosion Scenarios by using a Mechanistic Approach: the Caesium Case
Available formats
×
×

Reply to: Submit a response

Please enter your response.

Your details

Please enter a valid email address.

Conflicting interests

Do you have any conflicting interests? *