Abstract
This work reports the thermodynamic characterizations of organometallic species as a vehicle for the rapid separation of volatile nuclear fission products via gas chromatography due to differences in adsorption enthalpy. Because adsorption and sublimation thermodynamics are linearly correlated, there is considerable motivation to determine sublimation enthalpies. A method of isothermal thermogravimetric analysis, TGA-MS and melting point analysis are employed on thirteen lanthanide 1,1,1,5,5,5-hexafluoroacetylacetone complexes to determine sublimation enthalpies. An empirical correlation is used to estimate adsorption enthalpies of lanthanide complexes on a quartz column from the sublimation data. Additionally, four chelates are characterized by SC-XRD, elemental analysis, FTIR and NMR.
Highlights
Chemical separations of rare earth (RE) elements are essential to the development of renewable energies, hybrid vehicles, personal electronics, and nuclear security
This work reports the thermodynamic characterizations of organometallic species as a vehicle for the rapid separation of volatile nuclear fission products via gas chromatography due to differences in adsorption enthalpy
A method of isothermal thermogravimetric analysis, Thermogravimetric analysis (TGA)-mass spectrometer (MS) and melting point analysis are employed on thirteen lanthanide 1,1,1,5,5,5hexafluoroacetylacetone complexes to determine sublimation enthalpies
Summary
Chemical separations of rare earth (RE) elements are essential to the development of renewable energies, hybrid vehicles, personal electronics, and nuclear security. There has been a movement to improve the ‘‘greenness’’ of reactions, in particular by aiming toward solvent-free reactions [1, 2]. This is readily accomplished using gas-phase separations. In addition to the possibility of commercialization, there is interest in improving rapid separations for the purposes of nuclear forensics as emphasized by the Nuclear Forensics and Attribution Act (NFAA) of 2010 [6]. The NFAA has called upon the scientific community to address gaps in nuclear forensics technology for the immediate mitigation of developments in nuclear terrorism. It is of interest to develop sample preparation methods that can reduce the time required to perform the separation while retaining equivalent accuracy and precision to the established methods
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