Leinders Gregory, Cardinaels Thomas, Binnemans Koen, Verwerft Marc
Belgian Nuclear Research Centre (SCK·CEN) , Institute for Nuclear Materials Science , Boeretang 200 , B-2400 Mol , Belgium.
KU Leuven , Department of Chemistry , Celestijnenlaan 200F , P.O. Box 2404, B-3001 Heverlee , Belgium.
Inorg Chem. 2018 Apr 2;57(7):4196-4204. doi: 10.1021/acs.inorgchem.8b00517. Epub 2018 Mar 22.
The thermochemical behavior of low-temperature oxidation in fine UO powders has been investigated by simultaneous thermogravimetric analysis and differential scanning calorimetry. The evaluation of the thermochemical and kinetic data reveals a complex interplay between different mechanisms. The initial reaction concerns the rapid chemisorption of oxygen gas onto the surface of UO grains, having an activation energy of only 13.1 ± 0.6 kJ mol. The subsequent oxidation at temperatures between 40 and 100 °C occurs first at the surface via a field-assisted mechanism, which progresses via domain growth into the bulk. At more elevated temperatures, thermally activated diffusion becomes the dominant mechanism.
通过同步热重分析和差示扫描量热法研究了UO细粉中低温氧化的热化学行为。热化学和动力学数据的评估揭示了不同机制之间的复杂相互作用。初始反应涉及氧气在UO颗粒表面的快速化学吸附,其活化能仅为13.1±0.6 kJ/mol。随后在40至100°C之间的温度下的氧化首先通过场辅助机制在表面发生,该机制通过畴生长向体相推进。在更高的温度下,热激活扩散成为主导机制。