A growing focus of nuclear and radiochemistry is in the area of post-detonation material analysis from both a synthesis and chemical standpoint. It is the focus of this work to concentrate on chemical analysis, particularly with regard to rapid separation of entrenched fission oxides, principally rare earth oxides. The focus of this work is to highlight recent efforts to use thermochromatography to perform separations of rare earth oxides. Prior to separations, the oxides are dissolved in acid then treated with a variety of ligands, including 1,1,1,5,5,5-hexalfuoroacetylacetone (Hfac), 6,6,7,7,8,8,8-heptafluoro-2,2-dimethyl-3,5-octanedione (Hfod) and 2,2,6,6-tetramethyl-3,5-heptanedione (Hdpm). The resulting compounds are easily volatilized, allowing for gas-phase separation which will permit rapid separation over conventional liquid-liquid or column methods. In order to perform these separations, a gas chromatography (GC) system has been connected to an inductively coupled plasma mass spectrometry time-of-flight mass spectrometer (ICP-TOF-MS) to be used as the detector. The GC will be used to heat and separate the compounds, and the ICP-TOF-MS will be used to detect the resulting fragments. As a result, the metal ions and the time of arrival can be simultaneously determined. Additionally, the isotopic information of the metal ions can be validated to allow for rapid comparison to the results of other nuclear forensics techniques, including gamma-ray analysis, thermal ionization mass spectrometry, and x-ray fluorescence. The initial results have shown the time required for these samples is less than 8 hours, including the dissolution and compound preparation, while the actual separations require less than 10 minutes to obtain elemental and isotopic composition. The results of the separations using the three aforementioned ligands will be discussed in terms of resolution and thermodynamic parameters. It is the focus of this work to introduce another technique to the nuclear forensics community that will allow for rapid separations and subsequent elemental and isotopic analysis.

Thermochromatographic separations of volatile rare earth compounds for nuclear forensics analysis

249th National Meeting (2015)

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