Irradiation-induced amorphization of UO2 films prepared by spraying-assisted combustion synthesis

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

doi:10.1016/j.apsusc.2022.154437

Irradiation-induced amorphization of UO₂ films prepared by spraying-assisted combustion synthesis

Journal Article · Tue Aug 02 00:00:00 EDT 2022 · Applied Surface Science

DOI:https://doi.org/10.1016/j.apsusc.2022.154437· OSTI ID:1894773

Dede, Stefania ^[1]; Manukyan, Khachatur V. ^[2]; Roach, Jordan M. ^[2]; Majumdar, Ashabari ^[2]; Burns, Peter C. ^[2]; Aprahamian, Ani ^[3]

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

Spraying-assisted combustion synthesis with uranyl nitrate – acetylacetone – 2-methoxyethanol solutions was used to prepare UO₂ films on an aluminum alloy substrate. The tuning of the spraying parameters and annealing temperatures allowed the preparation of UO₂ films with thicknesses varying from 10–300 nm and 5–10 nm UO₂ grain size. High-resolution electron microscopy and X-ray photoelectron spectroscopy showed that increasing the annealing temperature promotes Mg diffusion from the substrate into the films. The incorporation of Mg reduced the overall crystallinity of the films. The irradiation with Ar²⁺ ions (1.7 MeV energy and a fluence of 2 × 10¹⁶ ions/cm²) did not degrade the quality of the films. However, the Mg content significantly influenced the irradiation-induced restructuring of the UO₂ films. Irradiated films with low or no Mg content exhibit high crystallinity, and the UO₂/Al interfacial layer becomes highly porous. Films with higher Mg content are mostly amorphized after irradiation. The origin of irradiation-induced amorphization was related to the formation of Mg_yU_1-yO_2±x solid solutions. Chemically complex, pore-free, and amorphous Mg-Al-O film/substrate interfacial layers enable continuous Mg diffusion during irradiation. As a result, the gradual increase in Mg amounts triggers irradiation-induced precipitation of a crystalline MgO-rich phase within the amorphous films.

View Accepted Manuscript (DOE)

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

Sponsoring Organization:: U.S. National Science Foundation; USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: NA0003888; NA0004093

OSTI ID:: 1894773

Alternate ID(s):: OSTI ID: 2007792

Journal Information:: Applied Surface Science, Journal Name: Applied Surface Science Vol. 603; ISSN 0169-4332

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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