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Title: Nanoscale Spatially Resolved Mapping of Uranium Enrichment

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% 235U, 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:
 [1];  [1];  [2];  [2]; ORCiD logo [3]
  1. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). National Security Directorate
  2. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Energy and Environment Directorate
  3. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Physical and Computational Sciences Directorate
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA)
OSTI Identifier:
1562527
Report Number(s):
PNNL-SA-139895
Journal ID: ISSN 2045-2322
Grant/Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Scientific Reports
Additional Journal Information:
Journal Volume: 9; Journal Issue: 1; Journal ID: ISSN 2045-2322
Publisher:
Nature Publishing Group
Country of Publication:
United States
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 States: N. p., 2019. Web. doi:10.1038/s41598-019-48479-5.
Kautz, Elizabeth, Burkes, Douglas, Joshi, Vineet, Lavender, Curt, & Devaraj, Arun. Nanoscale Spatially Resolved Mapping of Uranium Enrichment. United States. doi:10.1038/s41598-019-48479-5.
Kautz, Elizabeth, Burkes, Douglas, Joshi, Vineet, Lavender, Curt, and Devaraj, Arun. Fri . "Nanoscale Spatially Resolved Mapping of Uranium Enrichment". United States. doi:10.1038/s41598-019-48479-5. https://www.osti.gov/servlets/purl/1562527.
@article{osti_1562527,
title = {Nanoscale Spatially Resolved Mapping of Uranium Enrichment},
author = {Kautz, Elizabeth and Burkes, Douglas and Joshi, Vineet and Lavender, Curt and Devaraj, Arun},
abstractNote = {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 nm3) of depleted and low-enriched U alloyed with 10 wt% molybdenum that has different nominal enrichments of 0.20 and 19.75% 235U, 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},
issn = {2045-2322},
number = 1,
volume = 9,
place = {United States},
year = {2019},
month = {8}
}

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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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