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:
-
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- 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:
- Journal Article: 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. 2018.
"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},
url = {https://www.osti.gov/biblio/1479934},
journal = {Spectrochimica Acta. Part B, Atomic Spectroscopy},
issn = {0584-8547},
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}
}
Web of Science
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
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
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
Analysis of nuclear materials by energy dispersive X-ray fluorescence and spectral effects of alpha decay
journal, July 2009
- Worley, Christopher G.
- Journal of Radioanalytical and Nuclear Chemistry, Vol. 282, Issue 2
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
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
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
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
Calculation methods for fluorescent x-ray spectrometry. Empirical coefficients versus fundamental parameters
journal, June 1968
- Criss, J. W.; Birks, L. S.
- Analytical Chemistry, Vol. 40, Issue 7
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