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The overall objectives of this project were to gain a fundamental understanding of the solubility and phase behavior of metal chelates in supercritical CO2. Extraction with CO2 is a excellent way to remove organic compounds from soils, sludges and aqueous solutions and recent research has demonstrated that together with chelating agents it is a viable way to remove metals, as well. In this project we sought to gain fundamental knowledge that is vital to computing phase behavior, and modeling and designing processes using CO2 to separate organics and metal compounds from DOE mixed wastes. Our overall program was a comprehensive one to measure, model and compute the solubility of metal chelate complexes in supercritical CO2 and CO2/cosolvent mixtures. One aspect of this work was the measurement of local solvation of metal chelates using UV-visible spectroscopy, which provided information on the solution microstructure. We also focused on the measurement of the solubility of met al chelates in supercritical CO2 and CO2/cosolvent mixtures, as well as the phase behavior of the chelating agents themselves in CO2. The purpose of these measurements was to provide information with which we could evaluate and develop thermodynamic models of the solubility behavior. Finally, we focused on the implementation of a more reliable computational technique, based on interval mathematics, to compute the phase equilibria using the thermodynamic models. These studies were undertaken because fundamental information about metal chelate solubility in supercritical CO2 is important in the design of processes using CO2 to extract components from mixed wastes and in determining the optimum operating conditions

Spectroscopy, Modeling and Computation of Metal Chelate Solubility in Supercritical CO2