Safely probing the chemistry of Chernobyl nuclear fuel using micro-focus X-ray analysis

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

doi:10.1039/d0ta09131f

Title: Safely probing the chemistry of Chernobyl nuclear fuel using micro-focus X-ray analysis

Journal Article · Wed Feb 10 00:00:00 EST 2021 · Journal of Materials Chemistry. A

DOI:https://doi.org/10.1039/d0ta09131f· OSTI ID:1777434

Ding, Hao ^[1];

^[1]; Gausse, Clémence ^[1];

^[1];

^[2];

^[3]; Nicholas, Sarah ^[3];

^[1];

^[1]

Univ. of Sheffield (United Kingdom). Dept. of Materials Science and Engineering, NucleUS Immobilisation Science Laboratory
Paul Scherrer Inst. (PSI), Villigen (Switzerland). Swiss Light Source
Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)

Detailed chemical analysis of the solidified molten fuel still residing in the stricken Chernobyl reactor unit 4 are inferred using multi-modal micro-focus X-ray analysis of a low-radioactivity proxy. A fascinating mixture of molten UO₂, nuclear fuel cladding, concrete, stainless steel and other nuclear reactor components, these materials behaved like lava, solidifying to form a complex, highly radioactive glass-ceramic. Using element-specific chemical probes (micro-X-ray fluorescence and X-ray absorption spectroscopy), coupled with micro-diffraction analysis, the crystalline phase assemblage of simulants of these heterogeneous materials was established, which included “chernobylite” and a range of compositions in the (U_1-xZr_x)O₂ solid solution. Novel insight to nuclear accident fuel chemistry was obtained by establishing the oxidation state and local coordination of uranium not only in these crystalline phases, but uniquely in the amorphous fraction of the material, which varied depending on the history of the nuclear lava as it flowed through the reactor. This study demonstrates that micro-focus X-ray analysis of very small fractions of material can yield rich chemical information, which can be applied to nuclear-melt down materials to aid decommissioning and nuclear fuel management at nuclear accident sites.

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

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); UK Engineering and Physical Science Research Council (EPSRC)

Grant/Contract Number:: SC0012704; EP/N017374/1; EP/R01924X/1; EP/S020659/1

OSTI ID:: 1777434

Report Number(s):: BNL-221259-2021-JAAM; TRN: US2209452

Journal Information:: Journal of Materials Chemistry. A, Vol. 9, Issue 21; ISSN 2050-7488

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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