Molten uranium dioxide structure and dynamics

Skinner, L. B.; Parise, J. B.; Benmore, C. J.; Weber, J. K.R.; Williamson, M. A.; Tamalonis, A.; Hebden, A.; Wiencek, T.; Alderman, O. L.G.; Guthrie, M.; Leibowitz, L.

doi:10.1126/science.1259709

Molten uranium dioxide structure and dynamics

Journal Article · Fri Nov 21 00:00:00 EST 2014 · Science

DOI:https://doi.org/10.1126/science.1259709· OSTI ID:1174101

Skinner, L. B. ^[1]; Parise, J. B. ^[2]; Benmore, C. J. ^[3]; Weber, J. K.R. ^[4]; Williamson, M. A. ^[3]; Tamalonis, A. ^[4]; Hebden, A. ^[3]; Wiencek, T. ^[3]; Alderman, O. L.G. ^[4]; Guthrie, M. ^[5]; Leibowitz, L. ^[3]

Argonne National Laboratory (ANL), Argonne, IL (United States); Stony Brook Univ., Stony Brook, NY (United States); Materials Development Inc., Arlington Heights, IL (United States)
Stony Brook Univ., Stony Brook, NY (United States)
Argonne National Laboratory (ANL), Argonne, IL (United States)
Materials Development Inc., Arlington Heights, IL (United States)
Carnegie Inst., Washington, DC (United States)

Uranium dioxide (UO₂) is the major nuclear fuel component of fission power reactors. A key concern during severe accidents is the melting and leakage of radioactive UO₂ as it corrodes through its zirconium cladding and steel containment. Yet, the very high temperatures (>3140 kelvin) and chemical reactivity of molten UO₂ have prevented structural studies. In this work, we combine laser heating, sample levitation, and synchrotron x-rays to obtain pair distribution function measurements of hot solid and molten UO₂. The hot solid shows a substantial increase in oxygen disorder around the lambda transition (2670 K) but negligible U-O coordination change. On melting, the average U-O coordination drops from 8 to 6.7 ± 0.5. Molecular dynamics models refined to this structure predict higher U-U mobility than 8-coordinated melts.

View Accepted Manuscript (DOE)

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

Sponsoring Organization:: USDOE Office of Science (SC)

OSTI ID:: 1174101

Alternate ID(s):: OSTI ID: 1210814
OSTI ID: 1229222
OSTI ID: 1385852
OSTI ID: 1393975

Report Number(s):: BNL--107388-2015-JA

Journal Information:: Science, Journal Name: Science Journal Issue: 6212 Vol. 346; ISSN 0036-8075

Publisher:: AAASCopyright Statement

Country of Publication:: United States

Language:: English

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