2 research outputs found
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
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
Automated Separation of Uranium and Plutonium from Environmental Swipe Samples for Multiple Collector Inductively Coupled Plasma Mass Spectrometry
A fully
automated method for the separation of low-concentration uranium from
plutonium in environmental swipe samples has been developed. The offline
chromatography system features renewable 1 mL Eichrom TEVA and UTEVA
column generation from bulk resin slurry. Discrete fractions of the
separated actinides are delivered into user defined vials for future
analysis. Clean room background levels were achieved outside of a
cleanroom environment with this method. Purification of uranium and
plutonium from various sample matrixes and at various concentrations
was successful. Major and minor isotope ratios for both elements were
measured via multiple collector inductively coupled plasma mass spectrometry
and were in good agreement with certified reference values. Validation
of the separation method was conducted on archived environmental samples
and agreed with values previously reported using standard column chemistry