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Speciation and Bioavailability Measurements of Environmental Plutonium Using Diffusion in Thin Films
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Assessing Gas-Phase Ion Reactivity of 50 Elements with NO and the Direct Application for 239Pu in Complex Matrices
Kirby P Hobbs1, Amanda D French1, Kali M Melby1
1Pacific Northwest National Laboratory, Richland, Washington 99352, United States.
Analytical Chemistry
|April 4, 2024
Summary
Nitric oxide (NO) in ICP-MS/MS effectively measures plutonium-239 in complex samples. This method removes interferences without prior chemical separation, crucial for nuclear forensics applications.
Area of Science:
- Analytical Chemistry
- Mass Spectrometry
- Nuclear Chemistry
Background:
- Inductively coupled plasma tandem mass spectrometry (ICP-MS/MS) requires careful selection of reaction gases to resolve analyte/interference pairs.
- Nitric oxide (NO) has shown promise as a reaction gas, but its reactivity across a wide range of elements and its application in complex matrices remain underexplored.
Purpose of the Study:
- To systematically investigate the reactivity of 50 elements with nitric oxide (NO) in ICP-MS/MS.
- To validate theoretical modeling of reaction enthalpies for screening potential reaction gases.
- To develop and demonstrate a method for quantifying plutonium-239 (Pu) in challenging environmental matrices using NO.
Main Methods:
- Investigated reactions of 50 elements with NO in an ICP-MS/MS setup.
- Utilized theoretical modeling of reaction enthalpies to predict and screen gas reactivity.
- Developed a method to measure Pu-239 by reacting it to form Pu-16O+, monitoring at m/z = 255.
- Validated the method using standard reference materials spiked with Pu-239 and U-238.
Main Results:
- Established periodic trends in metal cation reactivity with NO.
- Validated theoretical reaction enthalpy modeling as a predictive tool for gas selection.
- Successfully measured Pu-239 in the presence of uranium and matrix constituents without chemical separation.
- Achieved accurate Pu-239 measurements within 6% of spiked values in complex environmental matrices.
Conclusions:
- Nitric oxide is a versatile reaction gas for ICP-MS/MS, enabling the analysis of elements, including actinides like Pu-239.
- The developed method allows for direct measurement of Pu-239 in environmental samples relevant to nuclear forensics, bypassing complex sample preparation.
- This study provides a foundational dataset for NO reactivity and its application in advanced mass spectrometry techniques.
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