Study of acoustic cavitation near metal surfaces contaminated by uranium

Abstract : The dismantling of UNGG reactors produces large volumes of contaminated metallic materials. Among these, magnesium-based alloys which are known as highly reactive metals, have a high risk of corrosion and can generate hydrogen gas that can cause serious damages during storage. In order to reduce the volume of generated radioactive effluents and downgrade nuclear wastes, sonochemistry can be applied as an efficient technology for metallic surface decontamination. Sonochemistry deals with the effects of ultrasound waves on chemical reactions in solution. The effects observed in sonochemistry originate from the acoustic cavitation phenomenon, which is the nucleation, growth and rapid implosive collapse of gas and vapor filled microbubbles. Excited species and radicals can be generated in the formed plasma and light (sonoluminescence) is emitted. When the bubble collapse takes place in the vicinity of a solid surface, it produces violent shock waves and microjets directed towards the surface. These physical effects strongly contribute in ultrasonic cleaning, surface depassivation and decontamination.This study focuses on: 1) the cavitation behaviors near a solid surface; 2) the ultrasonic structuration of extended magnesium surfaces; 3) the ultrasonic decontamination of radioactive metal surfaces. The sonochemical activity is evaluated by measuring H2O2 yields, sonochemiluminescence distribution and sonoluminescence spectra. Surface structuration and decontamination effects are followed by means of SEM, EDS, FTIR, Raman, XRD, wetting behavior analysis, mass spectrometry and ICP-AES.The investigations reveal a strong ultrasonic frequency dependency of the cavitation activity and distribution and of the effects generated on the Mg samples. A homogeneous spatial repartition of sonochemical activity is observed at frequencies ≥ 100 kHz. Asymmetrical bubble collapse is found more likely to happen near the solid surface at high frequency ultrasound. A golf-ball like extended structure is observed at frequencies between 100 and 362 kHz. It is shown that such architectures result from the ultrasonically controlled dissolution of the Mg surface. Heterogeneous nucleation provided by the creation of defects by ultrasound and the release of H2 gas are supposed to be at the origin of the crater formation. Decontamination of radioactive surfaces of Mg and Mg alloys demonstrate rapid ultrasonic cleaning followed by a slow recontamination process which is due to the adsorption of brucite formed on the surfaces of Mg or its alloys.
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Ran Ji. Study of acoustic cavitation near metal surfaces contaminated by uranium. Other. Université Montpellier, 2018. English. ⟨NNT : 2018MONTS131⟩. ⟨tel-02282007⟩

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