An Atomic-Scale Understanding of UO2 Surface Evolution during Anoxic Dissolution

Popel, Aleksej J.; Spurgeon, Steven R.; Matthews, Bethany E.; Olszta, Matthew J.; Tan, Beng Thye; Gouder, Thomas; Eloiridi, Rachel; Buck, Edgar C.; Farnan, Ian

doi:10.1021/acsami.0c09611

An Atomic-Scale Understanding of UO₂ Surface Evolution during Anoxic Dissolution

Journal Article · Mon Aug 10 04:00:00 EDT 2020 · ACS Applied Materials and Interfaces

DOI:https://doi.org/10.1021/acsami.0c09611· OSTI ID:1672147

^[1]; ^[2]; Matthews, Bethany E. ^[2]; ^[2]; Tan, Beng Thye ^[1]; Gouder, Thomas ^[3]; Eloiridi, Rachel ^[3]; ^[2]; Farnan, Ian ^[1]

Univ. of Cambridge (United Kingdom)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
European Commission, Karlsruhe (Germany). Joint Research Centre

Our present understanding of surface dissolution of nuclear fuels such as uranium dioxide (UO₂) is limited by the use of non-local characterization techniques. In this paper, we discuss the use of state-of-the-art scanning transmission electron microscopy (STEM) to reveal atomic–scale changes occurring to UO₂ thin films subjected to anoxic dissolution in deionised water. No amorphisation of the UO₂ film surface during dissolution is observed, and dissolution occurs preferentially at surface reactive sites that present as surface pits which increase in size as the dissolution proceeds. Using a combination of STEM imaging modes, energy-dispersive X-ray spectroscopy (STEM-EDS), and electron energy loss spectroscopy (STEM-EELS), we investigate structural defects and oxygen passivation of the surface that originates from the filling of the octahedral interstitial site in the centre of the unit cells and its associated lattice contraction. Taken together, our results reveal complex pathways for both the dissolution and infiltration of solutions into UO₂ surfaces.

View Accepted Manuscript (DOE)

Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE Laboratory Directed Research and Development (LDRD) Program

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 1672147

Report Number(s):: PNNL-SA--152605

Journal Information:: ACS Applied Materials and Interfaces, Journal Name: ACS Applied Materials and Interfaces Journal Issue: 35 Vol. 12; ISSN 1944-8244

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY
TEM
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anoxic dissolution
passivation
secondary phases
surface oxidation

An Atomic-Scale Understanding of UO2 Surface Evolution during Anoxic Dissolution

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An Atomic-Scale Understanding of UO₂ Surface Evolution during Anoxic Dissolution