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

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

doi:10.1016/j.ijms.2024.117385

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

Journal Article · Wed Dec 04 23:00:00 EST 2024 · International Journal of Mass Spectrometry

DOI:https://doi.org/10.1016/j.ijms.2024.117385· OSTI ID:2518993

Shrestha, Suraj ^[1]; Goodwin, Joseph V. ^[1]; ^[2]; ^[1]

Clemson University, SC (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

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. Here, 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.

View Accepted Manuscript (DOE)

Research Organization:: University of Florida, Gainesville, FL (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA), Office of Defense Nuclear Security

Grant/Contract Number:: NA0004142; AC05-00OR22725

OSTI ID:: 2518993

Alternate ID(s):: OSTI ID: 3002688

Journal Information:: International Journal of Mass Spectrometry, Journal Name: International Journal of Mass Spectrometry Vol. 508; ISSN 1387-3806

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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