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, A.

doi:10.1016/j.apsusc.2022.154437

Cited by 5 publications

(8 citation statements)

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“…It is noteworthy that increasing the annealing temperature to 550 °C during the preparation of UO 2 /Al samples enables the selective oxidative diffusion of Mg into the UO 2 films. The process facilitates the formation of Mg y U 1– y O 2±x (0 ≤ y ≤ 0.33) solid solutions without long-range order. ,, Accelerated Mg diffusion suppresses the mixing of the Al 2 O 3 interlayer with the film, evidenced by XPS results showing little or no Al in the irradiated films. Low dose 40 Ar 2+ irradiation in our previous work showed complete amorphization of the film.…”

Section: Discussionmentioning

confidence: 99%

“…X-ray photoelectron spectroscopy (XPS) was used to analyze the near-surface composition and chemical states of the films. The details of the analysis are described in our previous work . CasaXPS software was used to analyze the spectra .…”

Section: Methodsmentioning

confidence: 99%

“…The details of the analysis are described in our previous work. 44 CasaXPS software was used to analyze the spectra. 48 The atomic percentage of each element in the samples was quantified using the CasaXPS software, considering relative sensitivity factors for each element.…”

Section: Preparation Of Thin Filmsmentioning

confidence: 99%

“…Interestingly, Al was not present after irradiation with a relatively lower dose (2 × 10 16 ions/cm 2 ), as presented in our previous work. 44 Figure 5 (right panel) shows XPS spectra acquired at different etching times for an irradiated sample prepared at 550 °C. The main difference between the two samples is that the samples prepared at 550 °C contain almost no Al but more Mg.…”

Section: Elemental Composition and Chemical Statesmentioning

confidence: 99%

“…Thin films of UO 2 are essential for understanding the mechanisms governing the structural changes that nuclear fuel undergoes during reactor operation. ,− ,− In particular, ion irradiation of thin films of UO 2 or analog (CeO 2 ) materials is a safe approach for modeling irradiation-induced structural changes. ,− Solution combustion synthesis (SCS) − coupled with electrospraying (or spin coating) − is one of the latest developments and the most straightforward method for preparing UO 2 films with tunable thicknesses. This process involves deposition of a thin layer of uranyl nitrate + acetylacetone + 2-methoxyethanol (or uranyl nitrate–glycine–water) solution on a substrate (e.g., aluminum), followed by 20 min of annealing at 350–550 °C.…”

Section: Introductionmentioning

confidence: 99%

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Irradiation-enhanced Interactions at UO₂/Al₂O₃/Al Interfaces

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Combustion synthesis is used to prepare thin UO 2 films on aluminum alloy substrates. This simple preparation method involves electrospraying uranyl nitrate + acetylacetone + 2methoxyethanol solution on the substrate, followed by a short annealing at 350 or 550 °C. The irradiation of films with a 40 Ar 2+ ion beam (energy of 1.7 MeV and fluences of 7.7 × 10 16 and 1.3 × 10 17 ions/cm 2 ) 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 Al 2 O 3 interfacial layer between the film and the substrate. Local thermal spikes from the incoming ions facilitate the irradiationinduced mixing of immiscible Al 2 O 3 and UO 2 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 Al 2 O 3 interlayer with the film but forms Mg y U 1−y O 2±x solid solutions during irradiation. Local thermal heating triggers the precipitation of a discontinuous crystalline MgO layer close to the film surface. 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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Section: Discussionmentioning

confidence: 99%

Section: Methodsmentioning

confidence: 99%