DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Automated Separation of Uranium and Plutonium from Environmental Swipe Samples for Multiple Collector Inductively Coupled Plasma Mass Spectrometry

Abstract

A fully automated method for the separation of low-concentration uranium from plutonium in environmental swipe samples has been developed. The offline chromatography system features renewable 1 mL Eichrom TEVA and UTEVA column generation from bulk resin slurry. Discrete fractions of the separated actinides are delivered into user defined vials for future analysis. Clean room background levels were achieved outside of a cleanroom environment with this method. Purification of uranium and plutonium from various sample matrixes and at various concentrations was successful. Major and minor isotope ratios for both elements were measured via multiple collector inductively coupled plasma mass spectrometry and were in good agreement with certified reference values. Lastly, validation of the separation method was conducted on archived environmental samples and agreed with values previously reported using standard column chemistry.

Authors:
ORCiD logo [1];  [1];  [1];  [1];  [1];  [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA)
OSTI Identifier:
1460201
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Analytical Chemistry
Additional Journal Information:
Journal Volume: 90; Journal Issue: 15; Journal ID: ISSN 0003-2700
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Automated Separations; TEVA; UTEVA; Uranium; Plutonium; ICP–MS; Environmental Samples

Citation Formats

Metzger, Shalina C., Ticknor, Brian W., Rogers, Kayron T., Bostick, Debra A., McBay, Eddy H., and Hexel, Cole R. Automated Separation of Uranium and Plutonium from Environmental Swipe Samples for Multiple Collector Inductively Coupled Plasma Mass Spectrometry. United States: N. p., 2018. Web. doi:10.1021/acs.analchem.8b02095.
Metzger, Shalina C., Ticknor, Brian W., Rogers, Kayron T., Bostick, Debra A., McBay, Eddy H., & Hexel, Cole R. Automated Separation of Uranium and Plutonium from Environmental Swipe Samples for Multiple Collector Inductively Coupled Plasma Mass Spectrometry. United States. https://doi.org/10.1021/acs.analchem.8b02095
Metzger, Shalina C., Ticknor, Brian W., Rogers, Kayron T., Bostick, Debra A., McBay, Eddy H., and Hexel, Cole R. Sun . "Automated Separation of Uranium and Plutonium from Environmental Swipe Samples for Multiple Collector Inductively Coupled Plasma Mass Spectrometry". United States. https://doi.org/10.1021/acs.analchem.8b02095. https://www.osti.gov/servlets/purl/1460201.
@article{osti_1460201,
title = {Automated Separation of Uranium and Plutonium from Environmental Swipe Samples for Multiple Collector Inductively Coupled Plasma Mass Spectrometry},
author = {Metzger, Shalina C. and Ticknor, Brian W. and Rogers, Kayron T. and Bostick, Debra A. and McBay, Eddy H. and Hexel, Cole R.},
abstractNote = {A fully automated method for the separation of low-concentration uranium from plutonium in environmental swipe samples has been developed. The offline chromatography system features renewable 1 mL Eichrom TEVA and UTEVA column generation from bulk resin slurry. Discrete fractions of the separated actinides are delivered into user defined vials for future analysis. Clean room background levels were achieved outside of a cleanroom environment with this method. Purification of uranium and plutonium from various sample matrixes and at various concentrations was successful. Major and minor isotope ratios for both elements were measured via multiple collector inductively coupled plasma mass spectrometry and were in good agreement with certified reference values. Lastly, validation of the separation method was conducted on archived environmental samples and agreed with values previously reported using standard column chemistry.},
doi = {10.1021/acs.analchem.8b02095},
journal = {Analytical Chemistry},
number = 15,
volume = 90,
place = {United States},
year = {Sun Jul 29 00:00:00 EDT 2018},
month = {Sun Jul 29 00:00:00 EDT 2018}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 29 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Strengthening IAEA safeguards through environmental sampling and analysis
journal, June 1998


Mass spectrometric analysis for nuclear safeguards
journal, January 2015

  • Boulyga, Sergei; Konegger-Kappel, Stefanie; Richter, Stephan
  • Journal of Analytical Atomic Spectrometry, Vol. 30, Issue 7
  • DOI: 10.1039/C4JA00491D

Uranium isotope analysis by MC-ICP-MS in sub-ng sized samples
journal, January 2016

  • Boulyga, Sergei F.; Koepf, Andreas; Konegger-Kappel, Stefanie
  • Journal of Analytical Atomic Spectrometry, Vol. 31, Issue 11
  • DOI: 10.1039/C6JA00238B

Radionuclide determination in environmental samples by inductively coupled plasma mass spectrometry
journal, August 2006

  • Lariviere, Dominic; Taylor, Vivien F.; Evans, R. Douglas
  • Spectrochimica Acta Part B: Atomic Spectroscopy, Vol. 61, Issue 8
  • DOI: 10.1016/j.sab.2006.07.004

Separation of actinides from spent nuclear fuel: A review
journal, November 2016


A review on solid phase extraction of actinides and lanthanides with amide based extractants
journal, May 2017


Separation and preconcentration of uranium from acidic media by extraction chromatography
journal, August 1992


Determination of plutonium concentration and its isotopic ratio in environmental materials by ICP-MS after separation using and extraction chromatography
journal, January 1999

  • Muramatsu, Yasuyuki; Uchida, Shigeo; Tagami, Keiko
  • Journal of Analytical Atomic Spectrometry, Vol. 14, Issue 5
  • DOI: 10.1039/a900071b

Sequential Injection Renewable Separation Column Instrument for Automated Sorbent Extraction Separations of Radionuclides
journal, December 1998

  • Egorov, Oleg; O'Hara, Matthew J.; Grate, Jay W.
  • Analytical Chemistry, Vol. 71, Issue 2
  • DOI: 10.1021/ac980623j

An automated chromatography procedure optimized for analysis of stable Cu isotopes from biological materials
journal, January 2016

  • Enge, T. Gabriel; Field, M. Paul; Jolley, Dianne F.
  • Journal of Analytical Atomic Spectrometry, Vol. 31, Issue 10
  • DOI: 10.1039/C6JA00120C

Automated Analysis of Radionuclides in Nuclear Waste:  Rapid Determination of 90 Sr by Sequential Injection Analysis
journal, January 1996

  • Grate, Jay W.; Strebin, Robert; Janata, Jiri
  • Analytical Chemistry, Vol. 68, Issue 2
  • DOI: 10.1021/ac950561m

Automated pressurized injection system for the separation of actinides by extraction chromatography
journal, August 2012

  • Guérin, Nicolas; Nadeau, Kenny; Potvin, Sabrina
  • Journal of Radioanalytical and Nuclear Chemistry, Vol. 295, Issue 3
  • DOI: 10.1007/s10967-012-2102-6

Automated solid phase extraction of theophylline by sequential injection on renewable column
journal, January 1998

  • Dockendorff, Brian; Holman, David A.; Christian, Gary D.
  • Analytical Communications, Vol. 35, Issue 11
  • DOI: 10.1039/a806471g

Automated extraction chromatographic separations of actinides using separation-optimized sequential injection techniques
journal, January 1999

  • Grate, Jay W.; Egorov, Oleg B.; Fiskum, Sandra K.
  • The Analyst, Vol. 124, Issue 8
  • DOI: 10.1039/a902579k

A rapid and efficient automated method for the sequential separation of plutonium and radiostrontium in seawater
journal, September 2014

  • Kim, Hyuncheol; Chung, Kun Ho; Jung, Yoonhee
  • Journal of Radioanalytical and Nuclear Chemistry, Vol. 304, Issue 1
  • DOI: 10.1007/s10967-014-3595-y

Design and performance of an automated radionuclide separator: Its application on the determination of 99Tc in groundwater
journal, November 2013


Sequential Injection Method for Rapid and Simultaneous Determination of 236 U, 237 Np, and Pu Isotopes in Seawater
journal, November 2013

  • Qiao, Jixin; Hou, Xiaolin; Steier, Peter
  • Analytical Chemistry, Vol. 85, Issue 22
  • DOI: 10.1021/ac402673p

Peer Reviewed: From Flow Injection to Bead Injection.
journal, April 1999

  • Ruzicka, Jaromir; Scampavia, Louis
  • Analytical Chemistry, Vol. 71, Issue 7
  • DOI: 10.1021/ac990293i

Fully automated chromatographic purification of Sr and Ca for isotopic analysis
journal, January 2015

  • Romaniello, S. J.; Field, M. P.; Smith, H. B.
  • Journal of Analytical Atomic Spectrometry, Vol. 30, Issue 9
  • DOI: 10.1039/C5JA00205B

Introduction to the Actinides
book, January 2006


Round-robins in the area of uranium and plutonium bulk analysis of environmental samples
journal, August 2012

  • Pointurier, Fabien; Williams, Ross W.; LaMont, Stephen P.
  • Journal of Radioanalytical and Nuclear Chemistry, Vol. 296, Issue 2
  • DOI: 10.1007/s10967-012-1985-6

Spectral interferences in the determination of trace elements in environmental materials by inductively coupled plasma atomic emission spectrometry
journal, July 1999


Works referencing / citing this record:

Development and comparison of two high accuracy methods for uranium concentration in nuclear fuel: ID-TIMS and K-edge densitometry
journal, July 2019

  • Quemet, Alexandre; Ruas, Alexandre; Esbelin, Eric
  • Journal of Radioanalytical and Nuclear Chemistry, Vol. 321, Issue 3
  • DOI: 10.1007/s10967-019-06670-y