The work contained in this thesis addresses the single and multicomponent adsorption of hydrocarbons in silicalite. Both experimental and numerical work is presented. Experimental measurements are made using a volumetric technique and many equilibrium adsorption studies are reported for the first time. Multicomponent adsorption studies have revealed several novel adsorption phenomena. Intermolecular interaction within silicalite has been probed using deuterium nuclear magnetic resonance (<SUP>2</SUP>H NMR) experiments. For the first time data are presented for both single and multicomponent adsorbates within the structure and the effect of co-adsorption upon molecular microdynamics is investigated. Incorporating <SUP>2</SUP>H NMR data obtained with the network model for the adsorbent in a numerical simulation known as Monte Carlo Lattice Dynamics, has enabled equilibrium predictions to be made for single and multicomponent adsorption. On comparison with the experimental data obtained the results achieved by Monte Carlo Lattice Dynamics are very good and demonstrate the strength of the simulation orthodoxy. Molecular mechanic simulations, together with data obtained from <SUP>2</SUP>H NMR and volumetric studies have also been used to probe the behaviour of the external surface of silicalite in the study of adsorbate uptake kinetics. Results indicate that a surface-moderated insertion can affect the uptake of a component from the gas phase and hence affect the gross adsorption uptake properties of the material. Binary component studies have also been performed in which the interplay between adsorbate surface mobility and molecular desorption rates can affect a separation between components.
| Identifer | oai:union.ndltd.org:bl.uk/oai:ethos.bl.uk:603712 |
| Date | January 2000 |
| Creators | Hargreaves, S. M. |
| Publisher | University of Cambridge |
| Source Sets | Ethos UK |
| Detected Language | English |
| Type | Electronic Thesis or Dissertation |
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