The effect of cerium, neodymium, and ytterbium doping on UO2 dissolution

Asmussen, Susan E.; Asmussen, R. M.; Goulet, A. P.; Shimskey, R. W.; Hanson, Brady D.

doi:10.1016/j.jnucmat.2024.154916

The effect of cerium, neodymium, and ytterbium doping on UO₂ dissolution

Journal Article · Sun Jan 14 00:00:00 EST 2024 · Journal of Nuclear Materials

DOI:https://doi.org/10.1016/j.jnucmat.2024.154916· OSTI ID:2409171

^[1]; ^[1]; Goulet, A. P. ^[1]; Shimskey, R. W. ^[1]; Hanson, Brady D. ^[1]

Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Here, the dissolution rate of spent nuclear fuel has been studied heavily to understand the impacts of a failed waste package scenario on potential radionuclide release from a geologic repository. Multiple countries have evaluated these scenarios in oxidizing and reducing environments respective to their relevant repository conditions. The repository environment (e.g., water chemistry, temperature, oxygen content) and the fuel itself (e.g., chemical content of the fuel) both heavily impact the dissolution rate of the spent fuel. This work examined the impact that rare earth element dopants (Ce, Nd, Yb) have on the fuel dissolution under repository relevant conditions with decreasing oxidizing conditions using a single pass flowthrough system. UO₂ samples were doped with Ce, Nd, or Yb with concentrations between 1 and 5 at%. The addition of dopants to the samples reduced the dissolution rates on most samples relative to pure UO₂ samples. Scoping experiments that occurred in a less oxidizing environment showed a reduction in dissolution rate compared to fully oxidizing conditions. The results within highlight the importance of dopant behavior in used fuel dissolution modeling.

View Accepted Manuscript (DOE)

Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE; USDOE Office of Nuclear Energy (NE), Nuclear Energy University Program (NEUP); USDOE Office of Nuclear Energy (NE), Office of Spent Fuel and Waste Disposition. Office of Spent Fuel and Waste Science and Technology

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 2409171

Alternate ID(s):: OSTI ID: 2368993

Report Number(s):: PNNL-SA--183605

Journal Information:: Journal of Nuclear Materials, Journal Name: Journal of Nuclear Materials Vol. 591; ISSN 0022-3115

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

References (36)

Fuel corrosion processes under waste disposal conditions Shoesmith, D.W. Journal of Nuclear Materials, Vol. 282, Issue 1, p. 1-31 https://doi.org/10.1016/S0022-3115(00)00392-5	journal	November 2000
Determination of dissolution rates of spent fuel in carbonate solutions under different redox conditions with a flow-through experiment Röllin, S.; Spahiu, K.; Eklund, U. -B Journal of Nuclear Materials, Vol. 297, Issue 3 https://doi.org/10.1016/S0022-3115(01)00645-6	journal	September 2001
Determination of the activation energy for the formation of U3O8 on UO2 McEachern, R. J.; Choi, J. W.; Kolár̃, M. Journal of Nuclear Materials, Vol. 249, Issue 1 https://doi.org/10.1016/S0022-3115(97)00189-X	journal	September 1997
The effect of rare-earth fission products on the rate of U3O8 formation on UO2 McEachern, R. J.; Doern, D. C.; Wood, D. D. Journal of Nuclear Materials, Vol. 252, Issue 1-2 https://doi.org/10.1016/S0022-3115(97)00286-9	journal	January 1998
Surface electrochemistry of UO2 in dilute alkaline hydrogen peroxide solutions Goldik, J. S.; Nesbitt, H. W.; Noël, J. J. Electrochimica Acta, Vol. 49, Issue 11 https://doi.org/10.1016/j.electacta.2003.11.029	journal	April 2004
The Combined Influence of Gadolinium Doping and Non-stoichiometry on the Structural and Electrochemical Properties of Uranium Dioxide Kim, Jandee; Lee, Jeongmook; Youn, Young-Sang Electrochimica Acta, Vol. 247 https://doi.org/10.1016/j.electacta.2017.07.023	journal	September 2017
Effect of metallic iron on the oxidative dissolution of UO2 doped with a radioactive alpha emitter in synthetic Callovian-Oxfordian groundwater Odorowski, Mélina; Jegou, Christophe; De Windt, Laurent Geochimica et Cosmochimica Acta, Vol. 219 https://doi.org/10.1016/j.gca.2017.08.043	journal	December 2017
The effect of pH on the anodic dissolution of SIMFUEL (UO2) Santos, B. G.; Noël, J. J.; Shoesmith, D. W. Journal of Electroanalytical Chemistry, Vol. 586, Issue 1 https://doi.org/10.1016/j.jelechem.2005.09.021	journal	January 2006
Effect of external gamma irradiation on dissolution of the spent UO2 fuel matrix Jégou, C.; Muzeau, B.; Broudic, V. Journal of Nuclear Materials, Vol. 341, Issue 1 https://doi.org/10.1016/j.jnucmat.2005.01.008	journal	May 2005
Oxidation and dissolution of UO2 in bicarbonate media: Implications for the spent nuclear fuel oxidative dissolution mechanism Giménez, J.; Clarens, F.; Casas, I. Journal of Nuclear Materials, Vol. 345, Issue 2-3 https://doi.org/10.1016/j.jnucmat.2005.06.003	journal	October 2005
Simulations of H2O2 concentration profiles in the water surrounding spent nuclear fuel Nielsen, Fredrik; Lundahl, Karin; Jonsson, Mats Journal of Nuclear Materials, Vol. 372, Issue 1 https://doi.org/10.1016/j.jnucmat.2007.01.279	journal	January 2008
H2O2 and radiation induced dissolution of UO2 and SIMFUEL pellets Nilsson, Sara; Jonsson, Mats Journal of Nuclear Materials, Vol. 410, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2011.01.020	journal	March 2011
Radiation induced dissolution of UO2 based nuclear fuel – A critical review of predictive modelling approaches Eriksen, Trygve E.; Shoesmith, David W.; Jonsson, Mats Journal of Nuclear Materials, Vol. 420, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2011.10.027	journal	January 2012
Instant release fraction and matrix release of high burn-up UO2 spent nuclear fuel: Effect of high burn-up structure and leaching solution composition Serrano-Purroy, D.; Clarens, F.; González-Robles, E. Journal of Nuclear Materials, Vol. 427, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2012.04.036	journal	August 2012
On the redox reactivity of doped UO2 pellets – Influence of dopants on the H2O2 decomposition mechanism Pehrman, Reijo; Trummer, Martin; Lousada, Cláudio M. Journal of Nuclear Materials, Vol. 430, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2012.06.016	journal	November 2012
Preparation, characterisation and dissolution of a CeO2 analogue for UO2 nuclear fuel Stennett, Martin C.; Corkhill, Claire L.; Marshall, Luke A. Journal of Nuclear Materials, Vol. 432, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2012.07.038	journal	January 2013
The effect of fuel chemistry on UO2 dissolution Casella, Amanda; Hanson, Brady; Miller, William Journal of Nuclear Materials, Vol. 476 https://doi.org/10.1016/j.jnucmat.2016.04.025	journal	August 2016
Effect of Ce doping on UO2 structure and its oxidation behavior Ha, Yeong-Keong; Lee, Jeongmook; Kim, Jong-Goo Journal of Nuclear Materials, Vol. 480 https://doi.org/10.1016/j.jnucmat.2016.08.026	journal	November 2016
Oxidation and anion lattice defect signatures of hypostoichiometric lanthanide-doped UO2 Olds, Travis A.; Karcher, Samuel E.; Kriegsman, Kyle W. Journal of Nuclear Materials, Vol. 530 https://doi.org/10.1016/j.jnucmat.2019.151959	journal	March 2020
Effect of added gadolinium oxide on the thermal air oxidation of uranium dioxide Scheele, Randall D.; Hanson, Brady D.; Casella, Andrew M. Journal of Nuclear Materials, Vol. 552 https://doi.org/10.1016/j.jnucmat.2021.153008	journal	August 2021
Roles of Radiolytic and Externally Generated H ₂ in the Corrosion of Fractured Spent Nuclear Fuel Liu, Nazhen; Wu, Linda; Qin, Zack Environmental Science & Technology, Vol. 50, Issue 22 https://doi.org/10.1021/acs.est.6b04167	journal	October 2016
Impact of Stoichiometry on the Mechanism and Kinetics of Oxidative Dissolution of UO₂ Induced by H₂O₂ and γ-Irradiation Kumagai, Yuta; Barreiro Fidalgo, Alexandre; Jonsson, Mats The Journal of Physical Chemistry C, Vol. 123, Issue 15 https://doi.org/10.1021/acs.jpcc.9b00862	journal	March 2019
Formation of Studtite during the Oxidative Dissolution of UO ₂ by Hydrogen Peroxide: A SFM Study Clarens, F.; de Pablo, J.; Díez-Pérez, I. Environmental Science & Technology, Vol. 38, Issue 24 https://doi.org/10.1021/es0492891	journal	December 2004
Radiation Induced Spent Nuclear Fuel Dissolution under Deep Repository Conditions Jonsson, Mats; Nielsen, Fredrik; Roth, Olivia Environmental Science & Technology, Vol. 41, Issue 20 https://doi.org/10.1021/es070832y	journal	October 2007
Reducing Uncertainties Affecting the Assessment of the Long-Term Corrosion Behavior of Spent Nuclear Fuel Fanghänel, Thomas; Rondinella, Vincenzo V.; Glatz, Jean-Paul Inorganic Chemistry, Vol. 52, Issue 7 https://doi.org/10.1021/ic302012c	journal	June 2012
Long-term storage of spent nuclear fuel Ewing, Rodney C. Nature Materials, Vol. 14, Issue 3 https://doi.org/10.1038/nmat4226	journal	February 2015
Raman and X-ray Studies of Uranium-Lanthanum-Mixed Oxides Before and After Air Oxidation Talip, Zeynep; Wiss, Thierry; Raison, Philippe E. Journal of the American Ceramic Society, Vol. 98, Issue 7 https://doi.org/10.1111/jace.13559	journal	March 2015
Influence of Trivalent-Dopants on the Structural and Electrochemical Properties of Uranium Dioxide (UO ₂ ) Razdan, Mayuri; Shoesmith, David W. Journal of The Electrochemical Society, Vol. 161, Issue 3 https://doi.org/10.1149/2.047403jes	journal	December 2013
The Electrochemical Reactivity of 6.0 wt% Gd-Doped UO ₂ in Aqueous Carbonate/Bicarbonate Solutions Razdan, Mayuri; Shoesmith, David W. Journal of The Electrochemical Society, Vol. 161, Issue 4 https://doi.org/10.1149/2.050404jes	journal	January 2014
Effect of alpha radiolysis on doped UO ₂ dissolution under reducing conditions Mennecart, Thierry; Grambow, Bernd; Fattahi, M. Radiochimica Acta, Vol. 92, Issue 9-11 https://doi.org/10.1524/ract.92.9.611.55010	journal	November 2004
Corrosion of commercial spent nuclear fuel. 1. Formation of studtite and metastudtite Hanson, Brady D.; McNamara, Bruce; Buck, Edgar C. Radiochimica Acta, Vol. 93, Issue 3 https://doi.org/10.1524/ract.93.3.159.61613	journal	January 2005
Corrosion of commercial spent nuclear fuel. 2. Radiochemical analyses of metastudtite and leachates McNamara, Bruce; Hanson, Brady D.; Buck, Edgar C. Radiochimica Acta, Vol. 93, Issue 3 https://doi.org/10.1524/ract.93.3.169.61615	journal	January 2005
Reexamining the Dissolution of Spent Fuel: A Comparison of Different Methods for Calculating Rates Hanson, Brady D.; Stout, Ray B. MRS Proceedings, Vol. 824 https://doi.org/10.1557/PROC-824-CC2.4	journal	January 2004
Initial Results From Dissolution Testing of Spent Fuel Under Acidic Conditions Hanson, Brady D.; Friese, Judah I.; Soderquist, Chuck Z. MRS Proceedings, Vol. 824 https://doi.org/10.1557/PROC-824-CC8.6	journal	January 2004
A kinetic study of the dissolution of uraninite Grandstaff, D. E. Economic Geology, Vol. 71, Issue 8 https://doi.org/10.2113/gsecongeo.71.8.1493	journal	December 1976
Geological Disposal of Nuclear Waste in Tuff: Yucca Mountain (USA) Swift, Peter N.; Bonano, Evaristo J. Elements, Vol. 12, Issue 4 https://doi.org/10.2113/gselements.12.4.263	journal	July 2016

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The effect of cerium, neodymium, and ytterbium doping on UO2 dissolution

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