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Title: Nanoscale Spatially Resolved Mapping of Uranium Enrichment

Abstract

Abstract Spatially resolved analysis of uranium (U) isotopes in small volumes of actinide-bearing materials is critical for a variety of technical disciplines, including earth and planetary sciences, environmental monitoring, bioremediation, and the nuclear fuel cycle. However, achieving subnanometer-scale spatial resolution for such isotopic analysis is currently a challenge. By using atom probe tomography—a three-dimensional nanoscale characterisation technique—we demonstrate unprecedented nanoscale mapping of U isotopic enrichment with high sensitivity across various microstructural interfaces within small volumes (~100 nm 3 ) of depleted and low-enriched U alloyed with 10 wt% molybdenum that has different nominal enrichments of 0.20 and 19.75% 235 U, respectively. We map enrichment in various morphologies of a U carbide phase, the adjacent γ-UMo matrix, and across interfaces (e.g., carbide/matrix, grain boundary). Results indicate the U carbides were formed during casting, rather than retained from either highly enriched or depleted U feedstock materials. The approach presented here can be applied to study nanoscale variations of isotopic abundances in the broad class of actinide-bearing materials, providing unique insights into their origins and thermomechanical processing routes.

Authors:
; ; ; ; ORCiD logo
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA)
OSTI Identifier:
1619551
Alternate Identifier(s):
OSTI ID: 1562527
Report Number(s):
PNNL-SA-139895
Journal ID: ISSN 2045-2322; 12302; PII: 48479
Grant/Contract Number:  
AC05-76RL01830
Resource Type:
Published Article
Journal Name:
Scientific Reports
Additional Journal Information:
Journal Name: Scientific Reports Journal Volume: 9 Journal Issue: 1; Journal ID: ISSN 2045-2322
Publisher:
Nature Publishing Group
Country of Publication:
United Kingdom
Language:
English
Subject:
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS; uranium enrichment; atom probe tomography (APT); low-enriched uranium; nuclear fuel

Citation Formats

Kautz, Elizabeth, Burkes, Douglas, Joshi, Vineet, Lavender, Curt, and Devaraj, Arun. Nanoscale Spatially Resolved Mapping of Uranium Enrichment. United Kingdom: N. p., 2019. Web. doi:10.1038/s41598-019-48479-5.
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Kautz, Elizabeth, Burkes, Douglas, Joshi, Vineet, Lavender, Curt, & Devaraj, Arun. Nanoscale Spatially Resolved Mapping of Uranium Enrichment. United Kingdom. https://doi.org/10.1038/s41598-019-48479-5
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Kautz, Elizabeth, Burkes, Douglas, Joshi, Vineet, Lavender, Curt, and Devaraj, Arun. Fri . "Nanoscale Spatially Resolved Mapping of Uranium Enrichment". United Kingdom. https://doi.org/10.1038/s41598-019-48479-5.
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@article{osti_1619551,
title = {Nanoscale Spatially Resolved Mapping of Uranium Enrichment},
author = {Kautz, Elizabeth and Burkes, Douglas and Joshi, Vineet and Lavender, Curt and Devaraj, Arun},
abstractNote = {Abstract Spatially resolved analysis of uranium (U) isotopes in small volumes of actinide-bearing materials is critical for a variety of technical disciplines, including earth and planetary sciences, environmental monitoring, bioremediation, and the nuclear fuel cycle. However, achieving subnanometer-scale spatial resolution for such isotopic analysis is currently a challenge. By using atom probe tomography—a three-dimensional nanoscale characterisation technique—we demonstrate unprecedented nanoscale mapping of U isotopic enrichment with high sensitivity across various microstructural interfaces within small volumes (~100 nm 3 ) of depleted and low-enriched U alloyed with 10 wt% molybdenum that has different nominal enrichments of 0.20 and 19.75% 235 U, respectively. We map enrichment in various morphologies of a U carbide phase, the adjacent γ-UMo matrix, and across interfaces (e.g., carbide/matrix, grain boundary). Results indicate the U carbides were formed during casting, rather than retained from either highly enriched or depleted U feedstock materials. The approach presented here can be applied to study nanoscale variations of isotopic abundances in the broad class of actinide-bearing materials, providing unique insights into their origins and thermomechanical processing routes.},
doi = {10.1038/s41598-019-48479-5},
journal = {Scientific Reports},
number = 1,
volume = 9,
place = {United Kingdom},
year = {2019},
month = {8}
}
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https://doi.org/10.1038/s41598-019-48479-5
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Cited by: 3 works
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Figures / Tables:

Figure 1 Figure 1: Microstructures of depleted and low-enriched U-10Mo alloys: Backscattered scanning electron microscope images of microstructural features in the nuclear fuel analysed via APT in (a) DU-10Mo and (b) LEU-10Mo. The arrows point towards carbides. Two distinct carbide morphologies are visible in these micrographs: coarse and fine. The scale barmore » in each micrograph is 20 μm long.« less
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