Low-temperature oxidation of fine UO2 powders: thermochemistry and kinetics

Gregory Leinders; Thomas Cardinaels; Koen Binnemans; Marc Verwerft

doi:10.1021/acs.inorgchem.8b00517

Low-temperature oxidation of fine UO2 powders: thermochemistry and kinetics

Gregory Leinders, Thomas Cardinaels, Koen Binnemans, Marc Verwerft

Research output › peer-review

Abstract

The thermochemical behavior of low-temperature oxidation in fine UO2 powders has been investigated by simultaneous thermogravimetric analysis and differential scanning calorimetry. 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 UO2 grains, having an activation energy of only 13.1 ± 0.6 kJ mol−1. Subsequent oxidation at temperatures between 40 °C 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.

Original language	English
Pages (from-to)	4196-4204
Number of pages	8
Journal	Inorganic Chemistry
Volume	57
DOIs	https://doi.org/10.1021/acs.inorgchem.8b00517
State	Published - 22 Mar 2018

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10.1021/acs.inorgchem.8b00517

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title = "Low-temperature oxidation of fine UO2 powders: thermochemistry and kinetics",

abstract = "The thermochemical behavior of low-temperature oxidation in fine UO2 powders has been investigated by simultaneous thermogravimetric analysis and differential scanning calorimetry. 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 UO2 grains, having an activation energy of only 13.1 ± 0.6 kJ mol−1. Subsequent oxidation at temperatures between 40 °C 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.",

keywords = "low temperature, owydation, UO2, powders, Themochemistry, Kinetics",

author = "Gregory Leinders and Thomas Cardinaels and Koen Binnemans and Marc Verwerft",

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year = "2018",

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doi = "10.1021/acs.inorgchem.8b00517",

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journal = "Inorganic Chemistry",

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T1 - Low-temperature oxidation of fine UO2 powders: thermochemistry and kinetics

AU - Leinders, Gregory

AU - Cardinaels, Thomas

AU - Binnemans, Koen

AU - Verwerft, Marc

N1 - Score=10

PY - 2018/3/22

Y1 - 2018/3/22

N2 - The thermochemical behavior of low-temperature oxidation in fine UO2 powders has been investigated by simultaneous thermogravimetric analysis and differential scanning calorimetry. 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 UO2 grains, having an activation energy of only 13.1 ± 0.6 kJ mol−1. Subsequent oxidation at temperatures between 40 °C 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.

AB - The thermochemical behavior of low-temperature oxidation in fine UO2 powders has been investigated by simultaneous thermogravimetric analysis and differential scanning calorimetry. 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 UO2 grains, having an activation energy of only 13.1 ± 0.6 kJ mol−1. Subsequent oxidation at temperatures between 40 °C 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.

KW - low temperature

KW - owydation

KW - UO2

KW - powders

KW - Themochemistry

KW - Kinetics

UR - http://ecm.sckcen.be/OTCS/llisapi.dll/open/29417044

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DO - 10.1021/acs.inorgchem.8b00517

M3 - Article

SN - 0020-1669

VL - 57

SP - 4196

EP - 4204

JO - Inorganic Chemistry

JF - Inorganic Chemistry

ER -