Chemical characterisation of degraded nuclear fuel analogues simulating the Fukushima Daiichi nuclear accident

Hao Ding; Clémence Gausse; Malin C.Dixon Wilkins; Lucy M. Mottram; Martin C. Stennett; Daniel Grolimund; Ryan Tappero; Sarah Nicholas; Shikuan Sun; Tomooki Shiba; C. Paraskevoulakos; Neil C. Hyatt; Claire L. Corkhill

doi:10.1038/s41529-022-00219-3

Chemical characterisation of degraded nuclear fuel analogues simulating the Fukushima Daiichi nuclear accident

Hao Ding
, Clémence Gausse
, Malin C.Dixon Wilkins
, Lucy M. Mottram
, Martin C. Stennett
, Daniel Grolimund
, Ryan Tappero
, Sarah Nicholas
, Shikuan Sun
, Tomooki Shiba
, C. Paraskevoulakos
, Neil C. Hyatt^*
, Claire L. Corkhill^*

^*Corresponding author for this work

Research output: Contribution to journal › Article (Academic Journal) › peer-review

4 Citations (Scopus)

Abstract

The Fukushima Daiichi accident generated degraded nuclear fuel material, mixed with other reactor components, known as molten core-concrete interaction (MCCI) material. Simulant MCCI material was synthesised, excluding highly radioactive fission products, containing depleted U, and incorporating Ce as a surrogate for Pu. Multi-modal µ-focus X-ray analysis revealed the presence of the expected suite of U-Zr-O containing minerals, in addition to crystalline silicate phases CaSiO₃, SiO₂-cristobalite and Ce-bearing percleveite, (Ce,Nd)₂Si₂O₇. The formation of perclevite resulted from reaction between the U-Zr-O-depleted Ce-Nd-O melt and the silicate (SiO₂) melt. It was determined that the majority of U was present as U⁴⁺, whereas Ce was observed to be present as Ce³⁺, consistent with the highly reducing synthesis conditions. A range of Fe-containing phases characterised by different average oxidation states were identified, and it is hypothesised that their formation induced heterogeneity in the local oxygen potential, influencing the oxidation state of Ce.

Original language	English
Article number	10
Number of pages	13
Journal	npj Materials Degradation
Volume	6
Issue number	1
DOIs	https://doi.org/10.1038/s41529-022-00219-3
Publication status	Published - 2 Feb 2022

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© 2022, The Author(s).

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Ding, H., Gausse, C., Wilkins, M. C. D., Mottram, L. M., Stennett, M. C., Grolimund, D., Tappero, R., Nicholas, S., Sun, S., Shiba, T., Paraskevoulakos, C., Hyatt, N. C., & Corkhill, C. L. (2022). Chemical characterisation of degraded nuclear fuel analogues simulating the Fukushima Daiichi nuclear accident. npj Materials Degradation, 6(1), Article 10. https://doi.org/10.1038/s41529-022-00219-3

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title = "Chemical characterisation of degraded nuclear fuel analogues simulating the Fukushima Daiichi nuclear accident",

abstract = "The Fukushima Daiichi accident generated degraded nuclear fuel material, mixed with other reactor components, known as molten core-concrete interaction (MCCI) material. Simulant MCCI material was synthesised, excluding highly radioactive fission products, containing depleted U, and incorporating Ce as a surrogate for Pu. Multi-modal µ-focus X-ray analysis revealed the presence of the expected suite of U-Zr-O containing minerals, in addition to crystalline silicate phases CaSiO3, SiO2-cristobalite and Ce-bearing percleveite, (Ce,Nd)2Si2O7. The formation of perclevite resulted from reaction between the U-Zr-O-depleted Ce-Nd-O melt and the silicate (SiO2) melt. It was determined that the majority of U was present as U4+, whereas Ce was observed to be present as Ce3+, consistent with the highly reducing synthesis conditions. A range of Fe-containing phases characterised by different average oxidation states were identified, and it is hypothesised that their formation induced heterogeneity in the local oxygen potential, influencing the oxidation state of Ce.",

author = "Hao Ding and Cl{\'e}mence Gausse and Wilkins, \{Malin C.Dixon\} and Mottram, \{Lucy M.\} and Stennett, \{Martin C.\} and Daniel Grolimund and Ryan Tappero and Sarah Nicholas and Shikuan Sun and Tomooki Shiba and C. Paraskevoulakos and Hyatt, \{Neil C.\} and Corkhill, \{Claire L.\}",

note = "Publisher Copyright: {\textcopyright} 2022, The Author(s).",

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doi = "10.1038/s41529-022-00219-3",

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Ding, H, Gausse, C, Wilkins, MCD, Mottram, LM, Stennett, MC, Grolimund, D, Tappero, R, Nicholas, S, Sun, S, Shiba, T, Paraskevoulakos, C, Hyatt, NC & Corkhill, CL 2022, 'Chemical characterisation of degraded nuclear fuel analogues simulating the Fukushima Daiichi nuclear accident', npj Materials Degradation, vol. 6, no. 1, 10. https://doi.org/10.1038/s41529-022-00219-3

TY - JOUR

T1 - Chemical characterisation of degraded nuclear fuel analogues simulating the Fukushima Daiichi nuclear accident

AU - Ding, Hao

AU - Gausse, Clémence

AU - Wilkins, Malin C.Dixon

AU - Mottram, Lucy M.

AU - Stennett, Martin C.

AU - Grolimund, Daniel

AU - Tappero, Ryan

AU - Nicholas, Sarah

AU - Sun, Shikuan

AU - Shiba, Tomooki

AU - Paraskevoulakos, C.

AU - Hyatt, Neil C.

AU - Corkhill, Claire L.

PY - 2022/2/2

Y1 - 2022/2/2

N2 - The Fukushima Daiichi accident generated degraded nuclear fuel material, mixed with other reactor components, known as molten core-concrete interaction (MCCI) material. Simulant MCCI material was synthesised, excluding highly radioactive fission products, containing depleted U, and incorporating Ce as a surrogate for Pu. Multi-modal µ-focus X-ray analysis revealed the presence of the expected suite of U-Zr-O containing minerals, in addition to crystalline silicate phases CaSiO3, SiO2-cristobalite and Ce-bearing percleveite, (Ce,Nd)2Si2O7. The formation of perclevite resulted from reaction between the U-Zr-O-depleted Ce-Nd-O melt and the silicate (SiO2) melt. It was determined that the majority of U was present as U4+, whereas Ce was observed to be present as Ce3+, consistent with the highly reducing synthesis conditions. A range of Fe-containing phases characterised by different average oxidation states were identified, and it is hypothesised that their formation induced heterogeneity in the local oxygen potential, influencing the oxidation state of Ce.

AB - The Fukushima Daiichi accident generated degraded nuclear fuel material, mixed with other reactor components, known as molten core-concrete interaction (MCCI) material. Simulant MCCI material was synthesised, excluding highly radioactive fission products, containing depleted U, and incorporating Ce as a surrogate for Pu. Multi-modal µ-focus X-ray analysis revealed the presence of the expected suite of U-Zr-O containing minerals, in addition to crystalline silicate phases CaSiO3, SiO2-cristobalite and Ce-bearing percleveite, (Ce,Nd)2Si2O7. The formation of perclevite resulted from reaction between the U-Zr-O-depleted Ce-Nd-O melt and the silicate (SiO2) melt. It was determined that the majority of U was present as U4+, whereas Ce was observed to be present as Ce3+, consistent with the highly reducing synthesis conditions. A range of Fe-containing phases characterised by different average oxidation states were identified, and it is hypothesised that their formation induced heterogeneity in the local oxygen potential, influencing the oxidation state of Ce.

UR - https://www.scopus.com/pages/publications/85124343105

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DO - 10.1038/s41529-022-00219-3

M3 - Article (Academic Journal)

AN - SCOPUS:85124343105

SN - 2397-2106

VL - 6

JO - npj Materials Degradation

JF - npj Materials Degradation

IS - 1

M1 - 10

ER -

Chemical characterisation of degraded nuclear fuel analogues simulating the Fukushima Daiichi nuclear accident

Abstract

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A Collaborative Database to Support the Ongoing Fukushima Daiichi NPP Decommissioning

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Chemical characterisation of degraded nuclear fuel analogues simulating the Fukushima Daiichi nuclear accident

Abstract

Bibliographical note

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A Collaborative Database to Support the Ongoing Fukushima Daiichi NPP Decommissioning

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