Initial Characterization and Optimization of the Liquid Sampling-Atmospheric Pressure Glow Discharge Ionization Source Coupled to an Orbitrap Mass Spectrometer for the Determination of Plutonium

Joseph V. Goodwin, Benjamin T. Manard, Brian W. Ticknor, Paula Cable-Dunlap, R. Kenneth Marcus

Research output: Contribution to journalArticlepeer-review

7 Scopus citations

Abstract

Plutonium measurements are essential to the nuclear forensics and safeguards community. The liquid sampling-atmospheric pressure glow discharge (LS-APGD) microplasma ionization source coupled with an Orbitrap mass spectrometer is a proven platform for uranium isotope ratio determinations. This work expands the LS-APGD-Orbitrap platform capabilities by reporting the first-ever analysis of plutonium with the LS-APGD and the first-ever measurement of elemental plutonium with an Orbitrap mass spectrometer. This coupling has the potential to dramatically reduce the complex sample manipulations required for traditional analysis techniques employed for actinide isotope ratio determinations. As a first step toward the goal of simultaneous uranium and plutonium isotope ratio determinations, the initial characterization and optimization of the platform for the detection of plutonium are reported. Collision-induced dissociation modality settings were optimized to reduce water-related and other molecular clusters containing plutonium, maximizing 242Pu16O2+ responses. A design of experiments study was conducted to optimize the discharge conditions of the dual-electrode LS-APGD toward the responsivity of 242Pu16O2+. The measurement sensitivity was determined from a Pu response curve, yielding a limit of detection of 10 fg (absolute) of total analyte when data was collected and processed with a Spectroswiss FTMS Booster X2 data acquisition system. Additionally, plutonium and uranium were measured in a simultaneous acquisition, and each analyte remained unaffected by the other. It is believed that the LS-APGD-Orbitrap platform could be a valuable addition to the nuclear forensics’ toolbox and, indeed, other scientific disciplines and regulatory communities in which rapid, high-resolution plutonium determinations are paramount.

Original languageEnglish
Pages (from-to)12131-12138
Number of pages8
JournalAnalytical Chemistry
Volume95
Issue number32
DOIs
StatePublished - Aug 15 2023

Funding

This work was supported by the Oak Ridge National Laboratory, managed by UT-Battelle for the Department of Energy under contract DE-AC05-000R22725. This work was funded by the United States National Nuclear Security Administration’s Office of Defense Nuclear Nonproliferation Research & Development. The authors would like to thank Dr. Brian Powell of Clemson University, Department of Environmental Engineering & Earth Sciences, for his assistance in handling plutonium.

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