Development of a Field-Deployable Mass Spectrometry System for Nuclear Forensics Applications Using Liquid...

There is a need for in-field actinide measurements in support of nuclear forensic, safeguards, and environmental monitoring missions. Traditional methods of inorganic/elemental analysis, such as inductively coupled plasma mass spectrometry (ICP-MS), have high operational overheads, making these platforms ill-suited for this task. The liquid sampling-atmospheric pressure glow discharge (LS-APGD) ionization source is a proven microplasma ionization source with significantly reduced operational overhead as compared to ICP-MS; however, most studies to date have focused on coupling the LS-APGD to an ultrahigh resolution Orbitrap mass spectrometer. While the Orbitrap mass spectrometer is a benchtop instrument, it is quite complex with a large footprint and requires extremely low mass analyzer pressures. The Advion Expression^L compact mass spectrometer (CMS) is a compact, easily transported single quadrupole mass spectrometer platform that was previously coupled with the LS-APGD to measure multielement/metal solutions, albeit not actinides. To this end, this manuscript reports the optimization of the LS-APGD with the Advion Expression^L CMS mass spectrometer platform specifically for in-field actinide (uranium and thorium) measurements. This is the first report on the optimization of the dual-electrode LS-APGD on the CMS, including a modified ion sampling geometry. This also includes the first analysis of thorium using the LS-APGD, regardless of mass spectrometer coupling. After establishing that the LS-APGD and the mass spectrometer operations could be optimized independently, the LS-APGD discharge conditions were optimized with a design of experiments approach, with the mass spectrometer parameters optimized by a full factorial study. Once fully optimized, limits of detection of 0.2 ng total analyte mass were found for both uranium and thorium, below the EPA requirements for drinking water.