A response surface model of morphological changes in UO₂ and U₃O₈ following high temperature aging

Adam M. Olsen; Ian Schwerdt; Alex Jolley; Nick Halverson; Bryony Richards; Luther W. McDonald IV

doi:10.1515/ract-2018-3040

Abstract

The morphological changes that take place during the processing and storage of uranium oxides can provide valuable information on the processing history and storage conditions of an interdicted sample. In this study microstructural changes in two uranium oxides (UO₂ and U₃O₈) due to changes in the aging conditions at elevated temperatures were quantified and modeled using a response surface methodology approach. This allowed the morphological changes to be used as a signature for the aging conditions for nuclear forensic analysis. A Box-Behnken design of experiment was developed using the independent variables: temperature from 100 to 400 °C, aging times from 2 to 48 h, and partial pressure of O2(PO2) between ~0.0 kPa and 21.3 kPa. The design of experiment consisted of 54 samples per uranium oxide. Each aged sample was characterized using scanning electron microscopy (SEM) for image analysis. Utilizing the Morphological Analysis for Materials (MAMA) software package, particle size and shape were quantified using the acquired SEM images. Analysis of the particle attributes was completed using the Kolmogorov–Smirnov two sample test (K–S test) to determine if the particle size and shape distributions were statistically distinct. This data was then used to create response surfaces of the quantitative morphological changes based on the developed design of experiment. The U₃O₈ samples showed no statistically quantifiable differences due to the aging conditions. However, the UO₂ samples had distinct morphological changes due to the experimental aging conditions. Specifically, the temperature factor had an increasing effect on the particle area, and a decreasing effect on particle circularity.

Keywords: Quantitative microscopy; nuclear forensics; electron microscopy; uranium oxides; response surface methodology

Funding source: U.S. Department of Homeland Security

Award Identifier / Grant number: 2015-DN-077-ARI092

Funding source: Defense Threat Reduction Agency

Award Identifier / Grant number: HDTRA1-16-1-0026

Funding statement: This work is supported by the U.S. Department of Homeland Security, Domestic Nuclear Detection Office, Funder Id: http://dx.doi.org/10.13039/100000180, under Grant Award Number 2015-DN-077-ARI092, Defense Threat Reduction Agency, Funder Id: http://dx.doi.org/10.13039/100000774, Grant Number: HDTRA1-16-1-0026. The views and conclusions contained in this document are those of the authors and should not be interpreted as necessarily representing the official policies, either expressed or implied, of the U.S. Department of Homeland Security. This work made use of University of Utah Shared facilities of the Surface Analysis and Nanoscale Imaging Group sponsored by the College of Engineering, Health Sciences Center, Office of the Vice President for Research, and the Utah Science Technology and Research (USTAR) Initiative of the State of Utah.

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Supplementary Material

The online version of this article offers supplementary material (https://doi.org/10.1515/ract-2018-3040).

Received: 2018-08-03

Accepted: 2019-01-14

Published Online: 2019-04-22

Published in Print: 2019-06-26

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Supplementary Material

A response surface model of morphological changes in UO₂ and U₃O₈ following high temperature aging

Abstract

References

Supplementary Material

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