Irradiation-enhanced Interactions at UO2/Al2O3/Al Interfaces

Dede, Stefania; Manukyan, Khachatur V.; Roach, Jordan M.; Robertson, Daniel; Burns, Peter C.; Aprahamian, Ani

doi:10.1021/acs.jpcc.3c01155

Title: Irradiation-enhanced Interactions at UO₂/Al₂O₃/Al Interfaces

Journal Article · 11 May 2023 · Journal of Physical Chemistry. C

DOI: https://doi.org/10.1021/acs.jpcc.3c01155 · OSTI ID:2007787

^[1];

^[2]; Roach, Jordan M. ^[2]; Robertson, Daniel ^[2];

^[2]; Aprahamian, Ani ^[3]

University of Notre Dame, IN (United States); Texas A&M University, College Station, TX (United States)
University of Notre Dame, IN (United States)
University of Notre Dame, IN (United States); A. Alikhanyan National Science Laboratory of Armenia, Yerevan (Armenia)

Combustion synthesis is used to prepare thin UO₂ films on aluminum alloy substrates. This simple preparation method involves electrospraying uranyl nitrate + acetylacetone + 2-methoxyethanol solution on the substrate, followed by a short annealing at 350 or 550 °C. The irradiation of films with a ⁴⁰Ar²⁺ ion beam (energy of 1.7 MeV and fluences of 7.7 × 10¹⁶ and 1.3 × 10¹⁷ ions/cm²) is conducted to investigate irradiation-induced restructuring processes. High-resolution transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS) investigations show that the annealing temperature significantly influences the crystallinity and stability of materials during irradiation. A small amount of Mg in the alloy substrate diffuses into the amorphous Al₂O₃ interfacial layer between the film and the substrate. Local thermal spikes from the incoming ions facilitate the irradiation-induced mixing of immiscible Al₂O₃ and UO₂ for the materials prepared at 350 °C. This mass diffusion produces relatively large cavities at the interface. Selective diffusion of a more significant amount of Mg for the materials prepared at 550 °C suppresses the mixing of the Al₂O₃ interlayer with the film but forms Mg_yU_1–yO_2±x solid solutions during irradiation. Local thermal heating triggers the precipitation of a discontinuous crystalline MgO layer close to the film surface. As a result, the enhanced and selective diffusion of Mg into the film makes the materials prepared at 550 °C more robust and mechanically stable than those prepared at 350 °C.

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Research Organization:: University of Notre Dame, IN (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA); National Science Foundation (NSF); US Army Research Office

Grant/Contract Number:: NA0004093; PHY-2011890; W911NF2110045

OSTI ID:: 2007787

Journal Information:: Journal of Physical Chemistry. C, Vol. 127, Issue 20; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Title: Irradiation-enhanced Interactions at UO2/Al2O3/Al Interfaces

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Title: Irradiation-enhanced Interactions at UO₂/Al₂O₃/Al Interfaces