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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/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.

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 Laboratory (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA), Office of Defense Nuclear Security
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. https://doi.org/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. https://doi.org/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 = {Mon Apr 30 00:00:00 EDT 2018},
month = {Mon Apr 30 00:00:00 EDT 2018}
}

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Works referenced in this record:

Analytical chemistry in nuclear technology
journal, January 1992

  • Ache, H. J.
  • Fresenius' Journal of Analytical Chemistry, Vol. 343, Issue 11
  • DOI: 10.1007/BF00328573

Determination of plutonium in nitric acid solutions using energy dispersive L X-ray fluorescence with a low power X-ray generator
journal, April 2015

  • Py, J.; Groetz, J. -E.; Hubinois, J. -C.
  • Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 780
  • DOI: 10.1016/j.nima.2015.01.073

Determination of uranium in process stream solutions from uranium extraction plant employing energy dispersive X-ray fluorescence spectrometry
journal, October 2011

  • Balaji Rao, Y.; Ramana, B. V. V.; Gayathri Raghavan, P.
  • Journal of Radioanalytical and Nuclear Chemistry, Vol. 294, Issue 3
  • DOI: 10.1007/s10967-011-1477-0

Analysis of nuclear materials by energy dispersive X-ray fluorescence and spectral effects of alpha decay
journal, July 2009


Development of a microanalytical energy dispersive X-ray fluorescence method for compositional characterization of (U, Pu)O 2 samples
journal, May 2017

  • Dhara, Sangita; Sanjay Kumar, S.; Jayachandran, Kavitha
  • Spectrochimica Acta Part B: Atomic Spectroscopy, Vol. 131
  • DOI: 10.1016/j.sab.2017.03.006

An EDXRF method for determination of uranium and thorium in AHWR fuel after dissolution
journal, March 2009

  • Dhara, Sangita; Kumar, S. Sanjay; Misra, N. L.
  • X-Ray Spectrometry, Vol. 38, Issue 2
  • DOI: 10.1002/xrs.1127

Low-Level Sulfur in Fuel Determination Using Monochromatic WD XRF—ASTM D 7039-04
journal, January 2005

  • Chen, Zw; Wei, F.; Radley, I.
  • Journal of ASTM International, Vol. 2, Issue 8
  • DOI: 10.1520/JAI12971

Determination of plutonium in spent nuclear fuel using high resolution X-ray
journal, August 2015

  • McIntosh, Kathryn G.; Reilly, Sean D.; Havrilla, George J.
  • Spectrochimica Acta Part B: Atomic Spectroscopy, Vol. 110
  • DOI: 10.1016/j.sab.2015.05.014

Calculation methods for fluorescent x-ray spectrometry. Empirical coefficients versus fundamental parameters
journal, June 1968


Works referencing / citing this record:

A direct and safe method for plutonium determination using total reflection X-ray fluorescence spectrometry
journal, January 2019

  • Dhara, Sangita; Sanyal, Kaushik; Paul, Sumana
  • Journal of Analytical Atomic Spectrometry, Vol. 34, Issue 2
  • DOI: 10.1039/c8ja00351c