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Thermospray Mass Spectrometry Ionization Processes: Fundamental Mechanisms for Speciation, Separation and Characterization of Organic Complexants in DOE Wastes

Description: The overall objective of this research was to develop and enhance our understanding of the identity of major organic complexant species and their products with metals in aqueous mixtures such as those found in DOE radioactive tank wastes. Our approach to achieving this objective was a series of incremental studies involving cooperative efforts at ORNL and at the University of Minnesota. Investigations at ORNL characterized soft ionization mass spectrometry processes for the complexant species by developing and interpreting positive and negative ion thermospray mass spectrometry (TMS) of some organic complexants and their decomposition products and relating the spectral distributions to gas phase chemistry. This knowledge of the gas phase chemistry can be related to known solution chemistry behavior. At the University of Minnesota liquid chromatography separations on zirconia-based chromatographic supports were studied in 2 order to understand the separation of organic complexants and the products formed by complexants with metals in complex aqueous mixtures. This information was used to define the conditions needed to introduce a simplified chemical stream into the mass spectrometer. Ultimately the knowledge gained from these parallel efforts were combined at ORNL to characterize the complexant species in a multi-component aqueous mixture. The final objective was to develop the analytical capability needed to identify complexant species and to define chemical equilibria for these species in DOE waste streams.
Date: December 31, 2001
Creator: Bostick, Debra T.; Caton, John E. & Carr, Mabbott, Gary
Partner: UNT Libraries Government Documents Department

Thermospray Mass Spectrometry Ionization Processes Fundamental Mechanisms for Speciation, Separation and Characterization of Organic Complexants in DOE Wastes

Description: The overall objective of this research is to develop and enhance our understanding of the chemical equilibria for major organic complexant species and their products with metals in aqueous mixtures such as those found in DOE radioactive tank wastes. Our approach to achieving this objective is a series of incremental studies involving cooperative efforts at Oak Ridge National Laboratory (ORNL) and at the University of Minnesota. Investigations at ORNL are characterizing soft ionization mass spectrometry processes for the complexant species by developing and interpreting positive and negative ion thermospray mass spectrometry (TMS) of some organic complexants and their decomposition products and relating the spectral distributions to gas phase chemistry. Subsequently this knowledge of the gas phase chemistry will be related to known solution chemistry behavior. At the University of Minnesota liquid chromatography separations on zirconia-based chromatographic supports are being studied in order to understand the separation of organic complexants and the products formed by complexants with metals in complex aqueous mixtures; and thereby define the conditions needed to introduce a simplified chemical stream into the mass spectrometer. Ultimately the knowledge gained from these parallel efforts will be combined at ORNL to characterize the complexant species in a multi-component aqueous mixture with the final objective being to develop the analytical capability needed to define chemical equilibria for complexant species in DOE waste streams.
Date: June 1, 1999
Creator: Caton, John E.; Bostick, Debra, T.; Carr, Peter W. & Mabbott, Gary
Partner: UNT Libraries Government Documents Department

Thermospray Mass Spectrometry Ionization Processes Fundamental Mechanisms for Speciation, Separation and Characterization of Organic complexants in DOE Wastes

Description: The overall objective is to develop and enhance our understanding of chemical equilibria for major organic complexant species (chelators, chelator fragments, small organic acids and their products) in multi-component aqueous matrices such as the mixtures of DOE stored wastes. To progress toward this objective, organic complexants must be separated and speciated in mixtures of high ionic strength. HPLC employing zirconia-based stationary phases is being studied in order to understand the separation requirements for organic complexants and the products formed by complexants with metals in complex aqueous mixtures. Separated complexant species will then be characterized using positive and negative ion thermospray mass spectrometry (TSMS). The final goal is to develop the analytical capability needed to define chemical concentration and equilibria for complexant species in DOE waste streams.
Date: June 1, 1999
Creator: Caton, John E.; Bostick, Debra T.; Carr, Peter W. & Mabbott, Gary
Partner: UNT Libraries Government Documents Department