Parametric optimization of the liquid sampling-atmospheric pressure glow discharge ionization source coupled to an Orbitrap mass spectrometer for neodymium isotope ratio determinations

Suraj Shrestha, Joseph V. Goodwin, Benjamin T. Manard, R. Kenneth Marcus

Research output: Contribution to journalArticlepeer-review

Abstract

Isotope ratio determinations are a valuable tool in several application areas. In nuclear forensics, the isotope ratios of uranium and plutonium are commonly used as a signature for the nuclear material's provenance and processing history. However, signatures from other coexisting elements, such as neodymium and samarium, can offer additional insights. The liquid sampling-atmospheric pressure glow discharge (LS-APGD) ionization source coupled to an Orbitrap mass spectrometer (MS) has demonstrated its utility for actinide measurements. This instrumental platform can leverage the high resolution offered by the Orbitrap MS to overcome potential isobaric interferences, such as 144Nd-144Sm, 148Nd-148Sm, and 150Nd-150Sm pairs. The work presented herein demonstrates the rapid, accurate, and precise determination of the isotope ratios for neodymium using the LS-APGD/Orbitrap MS. Both the LS-APGD and Orbitrap MS parameters were optimized systematically, with NdO+ found to be the most abundant, most reduced species after applying the optimal collision-induced dissociation modalities. A limit of detection of 3 pg of 142Nd was achieved when data was acquired and processed using the FTMS Booster, an external data acquisition and processing system offered by Spectroswiss. Excellent accuracy of better than 99 % and precision of <1 % RSD were achieved when a solution of the well-characterized neodymium standard (JNdi-1 standard) was analyzed under the optimized condition, indicating the LS-APGD/Orbitrap's great potential for isotope ratio analysis of Nd and other REEs for diverse applications.

Original languageEnglish
Article number117385
JournalInternational Journal of Mass Spectrometry
Volume508
DOIs
StatePublished - Feb 2025

Funding

This work was supported in-part 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\u2019s Office of Defense Nuclear Nonproliferation Research & Development. This work was also funded in-part by the Consortium for Nuclear Forensics under Department of Energy, National Nuclear Security Administration awards number DE-NA0004142. The authors declare the following financial interests/personal relationships which may be considered as potential competing interests: R. Kenneth Marcus reports financial support was provided by US Department of Energy. If there are other authors, they declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.This work was supported in-part 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. This work was also funded in-part by the Consortium for Nuclear Forensics under Department of Energy, National Nuclear Security Administration awards number DE-NA0004142.

Keywords

  • Isotope ratio mass spectrometry
  • LS-APGD
  • Microplasma
  • Neodymium
  • Orbitrap

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