4.7 Article

Mass spectrometric study of the laser-evaporated Fe-Zr-O system up to 3300 K

Journal

JOURNAL OF THE AMERICAN CERAMIC SOCIETY
Volume 105, Issue 3, Pages 2161-2170

Publisher

WILEY
DOI: 10.1111/jace.18185

Keywords

high temperatures; laser heating; mass spectrometry; vaporization; zirconia

Funding

  1. TCOFF
  2. TCOFF (Thermodynamic Characterisation of Fuel Debris and Fission Products) project

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The evaporation behavior of ZrO2 and Zr-Fe-O systems was investigated in this study using heating with laser pulses of millisecond duration and time-of-flight mass spectrometry. The findings suggest that evaporation of zirconia occurs in a noncongruent mode at temperatures above 3000 K, while the evaporation of the Zr-Fe-O system is greatly influenced by the fast evaporation of FeO.
Material systems such as U-Zr-O, Fe-Zr-O, and Zr-O have been recognized as fundamental for the analysis of in-vessel nuclear fuel debris behavior during a severe meltdown accident. In the present work, the evaporation behavior of ZrO2 and Zr-Fe-O systems are investigated using heating with laser pulses of millisecond duration and time-of-flight mass spectrometry. The relative partial pressures of main species of vapor over ZrO2 and ZrO2-FeO systems were measured at temperatures above 2750 K. The temperature dependence of O/Zr atomic ratio in vapor over zirconia was analyzed: it turned out that evaporation occurs in a noncongruent mode at temperatures above 3000 K. Evaporation of the Zr-Fe-O system was greatly affected by the fast evaporation of FeO, implying that the atomic Zr/Fe ratio, less than 0.1 below 3000 K, significantly increased with temperature. Moreover, the ratios of main vapor components were defined only by the surface temperature, independent of the zirconia sample origin.

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