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Title: Determination of plutonium in spent nuclear fuel using high resolution X-ray

Abstract

Characterization of Pu is an essential aspect of safeguards operations at nuclear fuel reprocessing facilities. A novel analysis technique called hiRX (high resolution X-ray) has been developed for the direct measurement of Pu in spent nuclear fuel dissolver solutions. hiRX is based on monochromatic wavelength dispersive X-ray fluorescence (MWDXRF), which provides enhanced sensitivity and specificity compared with conventional XRF techniques. A breadboard setup of the hiRX instrument was calibrated using spiked surrogate spent fuel (SSF) standards prepared as dried residues. Samples of actual spent fuel were utilized to evaluate the performance of the hiRX. The direct detection of just 39 ng of Pu is demonstrated. Initial quantitative results, with error of 4–27% and precision of 2% relative standard deviation (RSD), were obtained for spent fuel samples. The limit of detection for Pu (100 s) within an excitation spot of 200 μm diameter was 375 pg. This study demonstrates the potential for the hiRX technique to be utilized for the rapid, accurate, and precise determination of Pu. Moreover, the results highlight the analytical capability of hiRX for other applications requiring sensitive and selective nondestructive analyses.

Authors:
 [1];  [1];  [1]
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Publication Date:
Research Org.:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1312565
Alternate Identifier(s):
OSTI ID: 1249982
Report Number(s):
LA-UR-14-28020
Journal ID: ISSN 0584-8547
Grant/Contract Number:  
AC52-06NA25396
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Spectrochimica Acta. Part B, Atomic Spectroscopy
Additional Journal Information:
Journal Volume: 110; 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; analytical chemistry; XRF; hiRX; elemental analysis; elemental mapping; spent nuclear fuel

Citation Formats

McIntosh, Kathryn G., Reilly, Sean D., and Havrilla, George J. Determination of plutonium in spent nuclear fuel using high resolution X-ray. United States: N. p., 2015. Web. doi:10.1016/j.sab.2015.05.014.
McIntosh, Kathryn G., Reilly, Sean D., & Havrilla, George J. Determination of plutonium in spent nuclear fuel using high resolution X-ray. United States. doi:10.1016/j.sab.2015.05.014.
McIntosh, Kathryn G., Reilly, Sean D., and Havrilla, George J. Sat . "Determination of plutonium in spent nuclear fuel using high resolution X-ray". United States. doi:10.1016/j.sab.2015.05.014. https://www.osti.gov/servlets/purl/1312565.
@article{osti_1312565,
title = {Determination of plutonium in spent nuclear fuel using high resolution X-ray},
author = {McIntosh, Kathryn G. and Reilly, Sean D. and Havrilla, George J.},
abstractNote = {Characterization of Pu is an essential aspect of safeguards operations at nuclear fuel reprocessing facilities. A novel analysis technique called hiRX (high resolution X-ray) has been developed for the direct measurement of Pu in spent nuclear fuel dissolver solutions. hiRX is based on monochromatic wavelength dispersive X-ray fluorescence (MWDXRF), which provides enhanced sensitivity and specificity compared with conventional XRF techniques. A breadboard setup of the hiRX instrument was calibrated using spiked surrogate spent fuel (SSF) standards prepared as dried residues. Samples of actual spent fuel were utilized to evaluate the performance of the hiRX. The direct detection of just 39 ng of Pu is demonstrated. Initial quantitative results, with error of 4–27% and precision of 2% relative standard deviation (RSD), were obtained for spent fuel samples. The limit of detection for Pu (100 s) within an excitation spot of 200 μm diameter was 375 pg. This study demonstrates the potential for the hiRX technique to be utilized for the rapid, accurate, and precise determination of Pu. Moreover, the results highlight the analytical capability of hiRX for other applications requiring sensitive and selective nondestructive analyses.},
doi = {10.1016/j.sab.2015.05.014},
journal = {Spectrochimica Acta. Part B, Atomic Spectroscopy},
issn = {0584-8547},
number = C,
volume = 110,
place = {United States},
year = {2015},
month = {5}
}

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