Assessing Gas-Phase Ion Reactivity of 50 Elements with NO and the Direct Application for 239Pu in Complex Matrices Using ICP-MS/MS

Hobbs, Kirby P.; French, Amanda D.; Melby, Kali M.; Bylaska, Eric J.; Harouaka, Khadouja; Cox, Richard M.; Arnquist, Isaac J.; Beck, Chelsie L.

doi:10.1021/acs.analchem.3c04774

Title: Assessing Gas-Phase Ion Reactivity of 50 Elements with NO and the Direct Application for ²³⁹Pu in Complex Matrices Using ICP-MS/MS

Journal Article · Thu Apr 04 00:00:00 UTC 2024 · Analytical Chemistry

DOI: https://doi.org/10.1021/acs.analchem.3c04774 · OSTI ID:2405078

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^[1]; Melby, Kali M. ^[1];

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^[1]; Arnquist, Isaac J. ^[1];

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Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Understanding the reactivity of metal cations with various reaction gases in ICP-MS/MS is important to determine the best gas to use for a given analyte/interference pair. In this study, nitric oxide (NO) was investigated as the reaction gas following previous experimental designs. The reactions with 50 elements were investigated to examine periodic trends in reactivity, validate theoretical modeling of reaction enthalpies as a method to screen reactant gases, and provide a baseline for potential in-line gas separation methods. ICP-MS/MS studies involving actinides are typically limited to Th, U and Pu, with analyses of Np and Am rarely reported in the literature. To date, only two previous methods have investigated the use of NO in ICP-MS/MS analyses. To showcase the utility of NO, a method was developed to measure ²³⁹Pu in the presence of environmental matrix constituent and other actinides, like what could be expected from post-detonation debris, with no chemical separation prior to analysis. ²³⁹Pu⁺ was reacted to form ²³⁹Pu¹⁶O⁺, eliminating interferences derived from the sample matrix by measuring ²³⁹Pu⁺ intensity at m/z = 255 (²³⁹Pu¹⁶O⁺). To validate NO for ²³⁸U¹H⁺ interference removal in environmental matrices, standard reference materials were diluted to 1 mg per gram of solution and spiked to 0.05 pg/g of ²³⁹Pu and 1 µg/g ²³⁸U (Pu/U = 5 x 10^-8). Measured ²³⁹Pu concentrations were within 6% of the spiked value. In conclusion, these results demonstrate that reliable ²³⁹Pu measurements can be made at levels relevant to nuclear forensics without the need for extensive chemical matrix separation prior to analysis.

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Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: Office of the Deputy Assistant Secretary of Defense for Nuclear Matters; USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE National Nuclear Security Administration (NNSA), Office of Defense Nuclear Nonproliferation

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 2405078

Report Number(s):: PNNL-SA--191260

Journal Information:: Analytical Chemistry, Journal Name: Analytical Chemistry Journal Issue: 15 Vol. 96; ISSN 0003-2700

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Title: Assessing Gas-Phase Ion Reactivity of 50 Elements with NO and the Direct Application for 239Pu in Complex Matrices Using ICP-MS/MS

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Title: Assessing Gas-Phase Ion Reactivity of 50 Elements with NO and the Direct Application for ²³⁹Pu in Complex Matrices Using ICP-MS/MS