Elucidation of the Local Character of Chemical Reactivity through the Time-Resolved Chromatographic Analysis of Local Molecular Properties of Gaseous Molecules Adsorbed on Solid Surfaces

作者：Metaxa Eleni D^*

来源：Journal of Physical Chemistry C, 2011, 115(51): 25389-25412.

DOI：10.1021/jp2089824

The basic objective of this research work is to contribute to the understanding of "how adsorption processes could be used in the determination of Lennard-Jones parameters for gaseous molecules adsorbed on a solid surface, by means of the time-resolved analysis of molecular properties, such as polarizabilities, ionization energies, electron affinities, electro-negativities and hardness, which mirror the local character of chemical reactivity". To this end, the well-known methodology of reversed-flow inverse gas chromatography, which provides us with real experimental values for significant physicochemical quantities illustrating the adsorption-desorption phenomenon step by step, is appropriately associated with quantitative structure property relationship model and density functional theory. Finally, local molecular properties and Lennard-Jones parameters are determined for nine gas solid systems at 323.2 K, namely: C2H6(g)/TiO2(s), C2H4(g)/TiO2(s), C2H2(g)/TiO2(s), C2H6(g)/Fe2O3(s), C2H4(g)/Fe2O3(s), C2H2(g)/Fe2O3(s), C2H6(g)/ZnO(s), C2H4(g)/ZnO(s), and C2H2(g)/ZnO(s).

• 出版日期2011-12-29