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Title: Initial Benchmarking of the Liquid Sampling-Atmospheric Pressure Glow Discharge-Orbitrap System Against Traditional Atomic Mass Spectrometry Techniques for Nuclear Applications

Journal Article · · Journal of the American Society for Mass Spectrometry
 [1]; ; ; ;  [2]
  1. Clemson University, Department of Chemistry, Biosystems Research Complex (United States)
  2. Los Alamos National Laboratory, Chemistry Division – Actinide Analytical Chemistry (C-AAC) (United States)

The integration of the liquid sampling-atmospheric pressure glow discharge (LS-APGD) ion source with Orbitrap mass spectrometers has resulted in new opportunities in the field of isotope ratio mass spectrometry. In a field that has been dominated by thermal ionization mass spectrometry (TIMS) and inductively coupled plasma mass spectrometry (ICP-MS) on quadrupole and scanning-mode sector field analyzer platforms for highly accurate and precise measurements, the LS-APGD-Orbitrap system offers a benchtop instrument capable of meeting the rigorous International Target Values for measurement uncertainty for uranium (U). In order to benchmark the LS-APGD-Orbitrap, a series of U certified reference materials with increasing {sup 235}U isotopic composition were analyzed. By using U samples ranging in enrichment from 1 to 80%, the ability of the system to measure isotope ratios over a wide range is demonstrated. This analysis represents the first time that the LS-APGD-Orbitrap system has been used to analyze highly enriched U samples, allowing for the measurement of each of the U isotopes, including {sup 234}U and {sup 236}U-related species, which had not been achieved previously. Ultimately, the LS-APGD-Orbitrap system was able to measure CRM U-800 (assayed as {sup 235}U / {sup 238}U = 4.265622) as 4.266922, with a combined uncertainty, (u{sub c}), of 0.040%. These results are compared to those obtained using traditional elemental mass spectrometers including TIMS and ICP-MS-based instruments. The effectiveness of the LS-APGD-Orbitrap MS system for measuring U isotopes shows excellent promise in nuclear forensics, safeguards, and other nuclear weapon-based applications. .

OSTI ID:
22922909
Journal Information:
Journal of the American Society for Mass Spectrometry, Vol. 30, Issue 2; Other Information: Copyright (c) 2019 American Society for Mass Spectrometry; Country of input: International Atomic Energy Agency (IAEA); ISSN 1044-0305
Country of Publication:
United States
Language:
English