期刊
JOURNAL OF THE AMERICAN SOCIETY FOR MASS SPECTROMETRY
卷 30, 期 2, 页码 278-288出版社
SPRINGER
DOI: 10.1007/s13361-018-2071-2
关键词
Liquid sampling-atmospheric pressure glow discharge; Orbitrap; Isotope ratio mass spectrometry; Uranium; Nuclear forensics
资金
- Defense Threat Reduction Agency [HDTRA1-14-1-0010]
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 U-235 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 U-234 and U-236-related species, which had not been achieved previously. Ultimately, the LS-APGD-Orbitrap system was able to measure CRM U-800 (assayed as U-235 / U-238 = 4.265622) as 4.266922, with a combined uncertainty, (u(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. [GRAPHICS] .
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