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Title: Focused ion beam for improved spatially-resolved mass spectrometry and analysis of radioactive materials for uranium isotopic analysis

Abstract

The ability to acquire high-quality spatially-resolved mass spectrometry data is sought in many fields of study, but it often comes with high cost of instrumentation and a high level of expertise required. In addition, techniques highly regarded for isotopic analysis applications such as thermal ionization mass spectrometry (TIMS) don’t have the abil-ity to acquire spatially-resolved data. Another drawback is that for radioactive materials, which are often of interest for iso-topic analysis in geochemistry and nuclear forensics applications, high-end instruments often have restrictions on radioactivi-ty and non-dispersibility requirements. We have applied the use of a traditional microanalysis tool, the focused ion beam/scanning electron microscope (FIB/SEM), for preparation of radioactive materials either for direct analysis by spatially-resolved instruments such as secondary ion mass spectrometry (SIMS) and laser ablation inductively-coupled mass spec-trometry (LA-ICP-MS), or similarly to provide some level of spatial resolution to techniques that don’t inherently have that ability such as TIMS or quadrupole inductively coupled plasma mass spectrometry (Q-ICP-MS). We applied this preparation technique to various uranium compounds, which was especially useful for reducing sample sizes and ensuring non-dispersibility to allow for entry into non-rad or ultra-trace facilities. Our results show how this site-specific preparation can provide spatial context for nominallymore » bulk techniques such as TIMS and Q-ICP-MS. In addition, the analysis of samples extracted from a uranium dioxide fuel pellet via all methods, but especially NanoSIMS and LA-ICP-MS, showed enrichment heterogeneities that are important for nuclear forensics and are of interest for fuel performance.« less

Authors:
ORCiD logo; ; ; ; ; ; ; ; ;
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1582469
Alternate Identifier(s):
OSTI ID: 1597633
Report Number(s):
PNNL-SA-144768
Journal ID: ISSN 0039-9140; S0039914020300114; 120720; PII: S0039914020300114
Grant/Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article: Published Article
Journal Name:
Talanta
Additional Journal Information:
Journal Name: Talanta Journal Volume: 211 Journal Issue: C; Journal ID: ISSN 0039-9140
Publisher:
Elsevier
Country of Publication:
United Kingdom
Language:
English
Subject:
46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND TECHNOLOGY; Focused ion beam; Uranium; Isotopic analysis; Mass spectrometry; Spatial resolution

Citation Formats

Reilly, Dallas D., Beck, Chelsie L., Buck, Edgar C., Cliff, John B., Duffin, Andrew M., Lach, Timothy G., Liezers, Martin, Springer, Kellen WE., Tedrow, Stephanie J., and Zimmer, Mindy M. Focused ion beam for improved spatially-resolved mass spectrometry and analysis of radioactive materials for uranium isotopic analysis. United Kingdom: N. p., 2020. Web. doi:10.1016/j.talanta.2020.120720.
Reilly, Dallas D., Beck, Chelsie L., Buck, Edgar C., Cliff, John B., Duffin, Andrew M., Lach, Timothy G., Liezers, Martin, Springer, Kellen WE., Tedrow, Stephanie J., & Zimmer, Mindy M. Focused ion beam for improved spatially-resolved mass spectrometry and analysis of radioactive materials for uranium isotopic analysis. United Kingdom. https://doi.org/10.1016/j.talanta.2020.120720
Reilly, Dallas D., Beck, Chelsie L., Buck, Edgar C., Cliff, John B., Duffin, Andrew M., Lach, Timothy G., Liezers, Martin, Springer, Kellen WE., Tedrow, Stephanie J., and Zimmer, Mindy M. 2020. "Focused ion beam for improved spatially-resolved mass spectrometry and analysis of radioactive materials for uranium isotopic analysis". United Kingdom. https://doi.org/10.1016/j.talanta.2020.120720.
@article{osti_1582469,
title = {Focused ion beam for improved spatially-resolved mass spectrometry and analysis of radioactive materials for uranium isotopic analysis},
author = {Reilly, Dallas D. and Beck, Chelsie L. and Buck, Edgar C. and Cliff, John B. and Duffin, Andrew M. and Lach, Timothy G. and Liezers, Martin and Springer, Kellen WE. and Tedrow, Stephanie J. and Zimmer, Mindy M.},
abstractNote = {The ability to acquire high-quality spatially-resolved mass spectrometry data is sought in many fields of study, but it often comes with high cost of instrumentation and a high level of expertise required. In addition, techniques highly regarded for isotopic analysis applications such as thermal ionization mass spectrometry (TIMS) don’t have the abil-ity to acquire spatially-resolved data. Another drawback is that for radioactive materials, which are often of interest for iso-topic analysis in geochemistry and nuclear forensics applications, high-end instruments often have restrictions on radioactivi-ty and non-dispersibility requirements. We have applied the use of a traditional microanalysis tool, the focused ion beam/scanning electron microscope (FIB/SEM), for preparation of radioactive materials either for direct analysis by spatially-resolved instruments such as secondary ion mass spectrometry (SIMS) and laser ablation inductively-coupled mass spec-trometry (LA-ICP-MS), or similarly to provide some level of spatial resolution to techniques that don’t inherently have that ability such as TIMS or quadrupole inductively coupled plasma mass spectrometry (Q-ICP-MS). We applied this preparation technique to various uranium compounds, which was especially useful for reducing sample sizes and ensuring non-dispersibility to allow for entry into non-rad or ultra-trace facilities. Our results show how this site-specific preparation can provide spatial context for nominally bulk techniques such as TIMS and Q-ICP-MS. In addition, the analysis of samples extracted from a uranium dioxide fuel pellet via all methods, but especially NanoSIMS and LA-ICP-MS, showed enrichment heterogeneities that are important for nuclear forensics and are of interest for fuel performance.},
doi = {10.1016/j.talanta.2020.120720},
url = {https://www.osti.gov/biblio/1582469}, journal = {Talanta},
issn = {0039-9140},
number = C,
volume = 211,
place = {United Kingdom},
year = {Fri May 01 00:00:00 EDT 2020},
month = {Fri May 01 00:00:00 EDT 2020}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record at https://doi.org/10.1016/j.talanta.2020.120720

Citation Metrics:
Cited by: 11 works
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