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Title: Evaluation of high resolution X-ray monochromatic wavelength dispersive X-ray fluorescence instrument for determining Pu and U in nuclear reprocessing streams

Abstract

In this study, an alpha-prototype benchtop instrument was developed and tested for measuring Pu and U in spent fuel dissolver tanks in a nuclear fuel reprocessing plant. The high resolution X-ray (hiRX) instrument was designed with the aim of providing a new capability to measure samples with high radiation background with selectivity, accuracy, and precision using ultra-low volumes (7 μL) of liquid. The instrument was tested with specimens from the operational reprocessing facility at Savannah River National Laboratory. The results showed that bias was <6% for Pu nitrate process solution and < 18% for Pu in U/HNO 3 matrix. Instrumental precision was <1% RSD while between microcell repeatability was <6% RSD. The limit of detection for Pu in HNO 3 matrix was 3 × 10 -5 g/L (100 s, 35 W). Finally, this study demonstrates that hiRX technology has the potential to provide rapid and simultaneous quantification of Pu and U without sample preparation, making it suitable for process monitoring and materials control and accountability applications.

Authors:
ORCiD logo [1]; ORCiD logo [1];  [2];  [2]
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  2. Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL)
Publication Date:
Research Org.:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA), Office of Defense Nuclear Security (NA-70)
OSTI Identifier:
1479934
Alternate Identifier(s):
OSTI ID: 1564294
Report Number(s):
LA-UR-17-29121
Journal ID: ISSN 0584-8547
Grant/Contract Number:  
AC52-06NA25396; LA-UR-17-29121
Resource Type:
Accepted Manuscript
Journal Name:
Spectrochimica Acta. Part B, Atomic Spectroscopy
Additional Journal Information:
Journal Volume: 148; Journal Issue: C; Journal ID: ISSN 0584-8547
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS; MWDXRF; hiRX; Elemental analysis; Reprocessing; Accountancy

Citation Formats

McIntosh, Kathryn Gallagher, Havrilla, George Joseph, Gilmore Jr, Robert F., and Holland, Michael K. Evaluation of high resolution X-ray monochromatic wavelength dispersive X-ray fluorescence instrument for determining Pu and U in nuclear reprocessing streams. United States: N. p., 2018. Web. doi:10.1016/j.sab.2018.04.019.
McIntosh, Kathryn Gallagher, Havrilla, George Joseph, Gilmore Jr, Robert F., & Holland, Michael K. Evaluation of high resolution X-ray monochromatic wavelength dispersive X-ray fluorescence instrument for determining Pu and U in nuclear reprocessing streams. United States. doi:10.1016/j.sab.2018.04.019.
McIntosh, Kathryn Gallagher, Havrilla, George Joseph, Gilmore Jr, Robert F., and Holland, Michael K. Mon . "Evaluation of high resolution X-ray monochromatic wavelength dispersive X-ray fluorescence instrument for determining Pu and U in nuclear reprocessing streams". United States. doi:10.1016/j.sab.2018.04.019. https://www.osti.gov/servlets/purl/1479934.
@article{osti_1479934,
title = {Evaluation of high resolution X-ray monochromatic wavelength dispersive X-ray fluorescence instrument for determining Pu and U in nuclear reprocessing streams},
author = {McIntosh, Kathryn Gallagher and Havrilla, George Joseph and Gilmore Jr, Robert F. and Holland, Michael K.},
abstractNote = {In this study, an alpha-prototype benchtop instrument was developed and tested for measuring Pu and U in spent fuel dissolver tanks in a nuclear fuel reprocessing plant. The high resolution X-ray (hiRX) instrument was designed with the aim of providing a new capability to measure samples with high radiation background with selectivity, accuracy, and precision using ultra-low volumes (7 μL) of liquid. The instrument was tested with specimens from the operational reprocessing facility at Savannah River National Laboratory. The results showed that bias was <6% for Pu nitrate process solution and < 18% for Pu in U/HNO3 matrix. Instrumental precision was <1% RSD while between microcell repeatability was <6% RSD. The limit of detection for Pu in HNO3 matrix was 3 × 10-5 g/L (100 s, 35 W). Finally, this study demonstrates that hiRX technology has the potential to provide rapid and simultaneous quantification of Pu and U without sample preparation, making it suitable for process monitoring and materials control and accountability applications.},
doi = {10.1016/j.sab.2018.04.019},
journal = {Spectrochimica Acta. Part B, Atomic Spectroscopy},
number = C,
volume = 148,
place = {United States},
year = {2018},
month = {4}
}

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