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

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

doi:10.1038/s41529-022-00219-3

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

Journal Article · 01 February 2022 · npj Materials Degradation

DOI: https://doi.org/10.1038/s41529-022-00219-3 · OSTI ID:1886229

Ding, Hao ^[1]; Gausse, Clémence ^[1]; Wilkins, Malin Dixon ^[1]; Mottram, Lucy M. ^[1];

^[1];

^[2]; Tappero, Ryan ^[3];

^[3]; Sun, Shikuan ^[4]; Shiba, Tomooki ^[5]; Paraskevoulakos, C. ^[6];

^[1];

^[1]

University of Sheffield (United Kingdom)
Paul Scherrer Inst. (PSI), Villigen (Switzerland). Swiss Light Source
Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
University of Sheffield (United Kingdom); Foshan University (China)
Japan Atomic Energy Agency (JAEA), Tomioka Town (Japan)
University of Bristol (United Kingdom)

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.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); Engineering and Physical Science Research Council (EPSRC); Business, Energy & Industrial Strategy (BEIS)

Grant/Contract Number:: SC0012704

OSTI ID:: 1886229

Report Number(s):: BNL-223262-2022-JAAM

Journal Information:: npj Materials Degradation, Journal Name: npj Materials Degradation Journal Issue: 1 Vol. 6; ISSN 2397-2106

Publisher:: SpringerCopyright Statement

Country of Publication:: United States

Language:: English

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