Intermolecular potential energy functions for CO2 have been developed from first principles for use in heterogeneous systems, including one with explicit polarization. The intermolecular potentials have been expressed in a transferable form and parameterized from nearly exact electronic structure calculations. Models with and without explicit many-body polarization effects, known to be important in simulation of interfacial processes, are constructed. The models have been validated on pressure-density isotherms of bulk CO2 and adsorption in three metal-organic framework (MOF) materials. The present models appear to offer advantages over high quality fluid/liquid state potentials in describing CO2 interactions in interfacial environments where sorbates adopt orientations not commonly explored in bulk fluids. Thus, the nonpolar CO2-PHAST and polarizable CO2-PHAST* potentials are recommended for materials/interfacial simulations.
Identifer | oai:union.ndltd.org:USF/oai:scholarcommons.usf.edu:etd-6028 |
Date | 01 January 2013 |
Creators | Mullen, Ashley Lynn |
Publisher | Scholar Commons |
Source Sets | University of South Flordia |
Detected Language | English |
Type | text |
Format | application/pdf |
Source | Graduate Theses and Dissertations |
Rights | default |
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