Solution composition effects on the dissolution of a CeO2 analogue for UO2 and ThO2 nuclear fuels

Claire L. Corkhill; Martin C. Stennett; Neil C. Hyatt

doi:10.1557/opl.2015.334

Solution composition effects on the dissolution of a CeO₂ analogue for UO₂ and ThO₂ nuclear fuels

Claire L. Corkhill, Martin C. Stennett, Neil C. Hyatt

School of Earth Sciences

Research output: Chapter in Book/Report/Conference proceeding › Conference Contribution (Conference Proceeding)

5 Citations (Scopus)

Abstract

This study investigates the dissolution of CeO₂, an isostructural analogue for U02 and ThO₂, which was synthesized to closely approximate the microstructure of a spent nuclear fuel matrix. Dissolution of CeO₂ particles was performed in simplified solutions representative of saline, near-neutral and alkaline ground waters that may be encountered in geological disposal scenarios, and in acidic medium for comparison. The normalized mass loss of cerium was found to be significantly influenced by the formation of colloidal particles, especially in the near- neutral and alkaline solutions investigated. The normalized dissolution rate, RL(Ce), k (g m^-2 d^-1, in these two solutions was found to be similar, but significantly lower than in a nitric acid medium. The activation energies based on the normalized release rate of cerium, at 40°C, 70°C and 90°C in each solution, were in the range of 24 ± 3 kJ mol^-1 to 27 ± 7 kJ mol', indicative of a surface-mediated dissolution mechanism. The mechanism of dissolution was postulated to be similar in each of the solutions investigated, and further work is proposed to investigate the role of carbonate on the CeO2 dissolution mechanism.

Original language	English
Title of host publication	Scientific Basis for Nuclear Waste Management XXXVIII
Editors	Stephane Gin, Robert Jubin, Eric Vance, Josef Matyas
Publisher	Materials Research Society
Pages	185-190
Number of pages	6
ISBN (Electronic)	9781605117218
DOIs	https://doi.org/10.1557/opl.2015.334
Publication status	Published - 2015
Event	2014 MRS Fall Meeting - Boston, United States Duration: 30 Nov 2014 → 5 Dec 2014

Publication series

Name	Materials Research Society Symposium Proceedings
Volume	1744
ISSN (Print)	0272-9172

Conference

Conference	2014 MRS Fall Meeting
Country/Territory	United States
City	Boston
Period	30/11/14 → 5/12/14

Bibliographical note

Publisher Copyright:
© 2015 Materials Research Society.

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10.1557/opl.2015.334

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Cite this

Corkhill, C. L., Stennett, M. C., & Hyatt, N. C. (2015). Solution composition effects on the dissolution of a CeO₂ analogue for UO₂ and ThO₂ nuclear fuels. In S. Gin, R. Jubin, E. Vance, & J. Matyas (Eds.), Scientific Basis for Nuclear Waste Management XXXVIII (pp. 185-190). (Materials Research Society Symposium Proceedings; Vol. 1744). Materials Research Society. https://doi.org/10.1557/opl.2015.334

Corkhill, Claire L. ; Stennett, Martin C. ; Hyatt, Neil C. / Solution composition effects on the dissolution of a CeO₂ analogue for UO₂ and ThO₂ nuclear fuels. Scientific Basis for Nuclear Waste Management XXXVIII. editor / Stephane Gin ; Robert Jubin ; Eric Vance ; Josef Matyas. Materials Research Society, 2015. pp. 185-190 (Materials Research Society Symposium Proceedings).

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title = "Solution composition effects on the dissolution of a CeO2 analogue for UO2 and ThO2 nuclear fuels",

abstract = "This study investigates the dissolution of CeO2, an isostructural analogue for U02 and ThO2, which was synthesized to closely approximate the microstructure of a spent nuclear fuel matrix. Dissolution of CeO2 particles was performed in simplified solutions representative of saline, near-neutral and alkaline ground waters that may be encountered in geological disposal scenarios, and in acidic medium for comparison. The normalized mass loss of cerium was found to be significantly influenced by the formation of colloidal particles, especially in the near- neutral and alkaline solutions investigated. The normalized dissolution rate, RL(Ce), k (g m-2 d-1, in these two solutions was found to be similar, but significantly lower than in a nitric acid medium. The activation energies based on the normalized release rate of cerium, at 40°C, 70°C and 90°C in each solution, were in the range of 24 ± 3 kJ mol-1 to 27 ± 7 kJ mol', indicative of a surface-mediated dissolution mechanism. The mechanism of dissolution was postulated to be similar in each of the solutions investigated, and further work is proposed to investigate the role of carbonate on the CeO2 dissolution mechanism.",

author = "Corkhill, {Claire L.} and Stennett, {Martin C.} and Hyatt, {Neil C.}",

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doi = "10.1557/opl.2015.334",

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Corkhill, CL, Stennett, MC & Hyatt, NC 2015, Solution composition effects on the dissolution of a CeO₂ analogue for UO₂ and ThO₂ nuclear fuels. in S Gin, R Jubin, E Vance & J Matyas (eds), Scientific Basis for Nuclear Waste Management XXXVIII. Materials Research Society Symposium Proceedings, vol. 1744, Materials Research Society, pp. 185-190, 2014 MRS Fall Meeting, Boston, United States, 30/11/14. https://doi.org/10.1557/opl.2015.334

Solution composition effects on the dissolution of a CeO₂ analogue for UO₂ and ThO₂ nuclear fuels. / Corkhill, Claire L.; Stennett, Martin C.; Hyatt, Neil C.
Scientific Basis for Nuclear Waste Management XXXVIII. ed. / Stephane Gin; Robert Jubin; Eric Vance; Josef Matyas. Materials Research Society, 2015. p. 185-190 (Materials Research Society Symposium Proceedings; Vol. 1744).

Research output: Chapter in Book/Report/Conference proceeding › Conference Contribution (Conference Proceeding)

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AU - Hyatt, Neil C.

PY - 2015

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N2 - This study investigates the dissolution of CeO2, an isostructural analogue for U02 and ThO2, which was synthesized to closely approximate the microstructure of a spent nuclear fuel matrix. Dissolution of CeO2 particles was performed in simplified solutions representative of saline, near-neutral and alkaline ground waters that may be encountered in geological disposal scenarios, and in acidic medium for comparison. The normalized mass loss of cerium was found to be significantly influenced by the formation of colloidal particles, especially in the near- neutral and alkaline solutions investigated. The normalized dissolution rate, RL(Ce), k (g m-2 d-1, in these two solutions was found to be similar, but significantly lower than in a nitric acid medium. The activation energies based on the normalized release rate of cerium, at 40°C, 70°C and 90°C in each solution, were in the range of 24 ± 3 kJ mol-1 to 27 ± 7 kJ mol', indicative of a surface-mediated dissolution mechanism. The mechanism of dissolution was postulated to be similar in each of the solutions investigated, and further work is proposed to investigate the role of carbonate on the CeO2 dissolution mechanism.

AB - This study investigates the dissolution of CeO2, an isostructural analogue for U02 and ThO2, which was synthesized to closely approximate the microstructure of a spent nuclear fuel matrix. Dissolution of CeO2 particles was performed in simplified solutions representative of saline, near-neutral and alkaline ground waters that may be encountered in geological disposal scenarios, and in acidic medium for comparison. The normalized mass loss of cerium was found to be significantly influenced by the formation of colloidal particles, especially in the near- neutral and alkaline solutions investigated. The normalized dissolution rate, RL(Ce), k (g m-2 d-1, in these two solutions was found to be similar, but significantly lower than in a nitric acid medium. The activation energies based on the normalized release rate of cerium, at 40°C, 70°C and 90°C in each solution, were in the range of 24 ± 3 kJ mol-1 to 27 ± 7 kJ mol', indicative of a surface-mediated dissolution mechanism. The mechanism of dissolution was postulated to be similar in each of the solutions investigated, and further work is proposed to investigate the role of carbonate on the CeO2 dissolution mechanism.

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PB - Materials Research Society

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