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Rapid paper spray mass spectrometry characterization of uranium and exemplar molecular species

Journal Article · · Rapid Communications in Mass Spectrometry
DOI:https://doi.org/10.1002/rcm.8517· OSTI ID:1558286
 [1];  [2];  [1];  [1];  [1];  [1]
  1. Savannah River National Lab., Aiken, SC (United States)
  2. JEOL USA, Inc., Peabody, MA (United States)
+ Show Author Affiliations
The ability to detect and quantify the presence of specific inorganic elements and complexes is essential for environmental monitoring and nuclear safeguards applications. In this work, paper spray ionization mass spectrometry (PSI–MS) was used for the rapid chemical and isotopic characterization of trace inorganic species collected on cotton swipe substrates. Here, the direct analysis of cotton swipes using this ambient ionization technique led to fast sample analysis that retained original chemical information of the source material with minimal sample preparation. Mass spectra were collected on an atmospheric pressure ionization, high–resolution mass spectrometer for solutions containing uranyl acetate, uranyl chloride, uranyl nitrate, and uranyl tri–n–butylphosphate (uranyl–TBP) complexes. Gadolinium nitrate was used as an internal standard for the quantitative analysis of uranium. To demonstrate the ability to characterize inorganic contaminants in the presence of uranium, a multi–element inorganic standard containing U, Bi, Pb, Cd, Fe, and Zn was deposited onto cotton substrates and directly analyzed without purification. All elements doped on the cotton substrate were detected with strong signal–to–noise (S/N) ratios (S/N~1000 for UO2+ on multi–element doped swipes) and high integrated intensities (>105 counts) from collection periods of approximately 1 min. Limits of detection were determined to be approximately 94 ng for UO2+ and uranyl acetate through the measurement of ppb level solutions. The rapid analysis of uranium and other inorganic–containing samples while still retaining original chemical information (e.g. uranyl complexation) was demonstrated. Qualitative detection and speciation were achieved in less than 1 min of analysis. For uranium isotopic quantitation, longer accumulations (>15 min) can be sustained to improve the accuracy of minor 235U isotopic abundance measurements to approximately 1% error.
Research Organization:
Savannah River National Lab (SRNL), Aiken, SC (United States)
Sponsoring Organization:
USDOE; USDOE Office of Environmental Management (EM)
Grant/Contract Number:
AC09-08SR22470
OSTI ID:
1558286
Alternate ID(s):
OSTI ID: 1572117
Report Number(s):
SRNL-STI--00225
Journal Information:
Rapid Communications in Mass Spectrometry, Journal Name: Rapid Communications in Mass Spectrometry Journal Issue: 22 Vol. 33; ISSN 0951-4198
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English

References (32)

Paper spray ionization for ambient inorganic analysis: Paper spray ionization for ambient inorganic analysis journal March 2014
Age determination of plutonium material in nuclear forensics by thermal ionisation mass spectrometry journal February 2000
Prospects for the introduction of wide area monitoring using environmental sampling for proliferation detection journal August 2012
Rapid quantification of TBP and TBP degradation product ratios by FTIR-ATR journal August 2012
Strengthening IAEA safeguards through environmental sampling and analysis journal June 1998
Trace element and U isotope analysis of uraninite and ore concentrate: Applications for nuclear forensic investigations journal September 2017
Direct isotope ratio analysis of individual uranium–plutonium mixed particles with various U/Pu ratios by thermal ionization mass spectrometry journal February 2015
Rapid measurement of tacrolimus in whole blood by paper spray-tandem mass spectrometry (PS-MS/MS) journal February 2015
Development of prototype nuclear forensics library for nuclear materials and radioisotopes in Japan Atomic Energy Agency journal December 2017
Electrospray ionization of uranyl-citrate complexes: Adduct formation and ion-molecule reactions in 3D ion trap and ion cyclotron resonance trapping instruments journal September 2007
The novel analysis of uranyl compounds by electrospray-ion mobility-mass spectrometry journal January 2013
Direct and rapid quantitation of ephedrines in human urine by paper spray ionization/high resolution mass spectrometry journal August 2016
Validation of gamma-ray detection techniques for safeguards monitoring at natural uranium conversion facilities
  • Dewji, S. A.; Lee, D. L.; Croft, S.
  • Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 823 https://doi.org/10.1016/j.nima.2016.03.069
journal July 2016
Uranium aerosols at a nuclear fuel fabrication plant: Characterization using scanning electron microscopy and energy dispersive X-ray spectroscopy journal May 2017
Use of an ion mobility spectrometer for detecting uranium compounds journal July 2018
Paper Spray and Extraction Spray Mass Spectrometry for the Direct and Simultaneous Quantification of Eight Drugs of Abuse in Whole Blood journal July 2014
Characterization of Actinides Complexed to Nuclear Fuel Constituents Using ESI-MS journal February 2016
Measurement of Uranium Isotopes in Particles of U 3 O 8 by Secondary Ion Mass Spectrometry–Single-Stage Accelerator Mass Spectrometry (SIMS–SSAMS) journal June 2016
Direct Analysis of Aerosolized Chemical Warfare Simulants Captured on a Modified Glass-Based Substrate by “Paper-Spray” Ionization journal September 2017
Paper Spray Ionization Coupled to High Resolution Tandem Mass Spectrometry for Comprehensive Urine Drug Testing in Comparison to Liquid Chromatography-Coupled Techniques after Urine Precipitation or Dried Urine Spot Workup journal October 2017
Highly Sensitive and Selective Uranium Detection in Natural Water Systems Using a Luminescent Mesoporous Metal–Organic Framework Equipped with Abundant Lewis Basic Sites: A Combined Batch, X-ray Absorption Spectroscopy, and First Principles Simulation Investigation journal March 2017
Theoretical Mechanism Study of UF 6 Hydrolysis in the Gas Phase (II) journal August 2009
Environmental monitoring of plutonium at ultratrace level in natural water (Sea of Galilee—Israel) by ICP-SFMS and MC-ICP-MS journal January 2004
Nuclear forensics—a methodology providing clues on the origin of illicitly trafficked nuclear materials journal January 2005
Mass spectrometric analysis for nuclear safeguards journal January 2015
Thermal ionisation mass spectrometry (TIMS) in nuclear science and technology – a review journal January 2016
Uranium isotope analysis by MC-ICP-MS in sub-ng sized samples journal January 2016
Analysis of human gliomas by swab touch spray-mass spectrometry: applications to intraoperative assessment of surgical margins and presence of oncometabolites journal January 2017
Drug screening method development for paper spray coupled to a triple quadrupole mass spectrometer journal January 2017
Considerations for uranium isotope ratio analysis by atmospheric pressure ionization mass spectrometry journal January 2019
Plutonium isotope ratio analysis at femtogram to nanogram levels by multicollector ICP-MS journal January 2001
Investigation of the isotopic composition of lead and of trace elements concentrations in natural uranium materials as a signature in nuclear forensics journal January 2007

Figures / Tables (8)

Table 1(p. 11)table Table 1
Table 2(p. 11)table Table 2
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Figure 6(p. 17)figure Figure 6

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Related Subjects

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND TECHNOLOGY
isotopic analysis
mass spectrometry
paper spray ionization
uranium detection
whole molecule detection