Model column structure for the analysis of the flow and band-broadening characteristics of silica monoliths

We report on the use of commercial computational fluid dynamics software to study the band broadening in a perfectly ordered three-dimensional model structure, the so-called tetrahedral skeleton column (TSC), selected for its close geometrical resemblance to the specific pore network topology of silica monoliths. Van Deemter plots are presented for the case of a species flow through a non-porous skeleton and for the case of a retained component (k' = 1) in a porous skeleton (mesopore porosity epsilon = 0.6 in both cases). Using the flow domain as the characteristic scaling dimension, the TSC model yields reduced plate heights as small as h(min) = 0.8 and separation impedances as small as E-min = 120 for a retained component with k' = 1. The very small reduced plate heights for the TSC model can without any doubt largely be attributed to the perfect homogeneity of the considered model structure: the B and C terms are similar to those obtained in real silica monoliths with similar external porosity, whereas the A term is significantly (about a factor of 10) smaller. The present study hence suggests that further experimental work to obtain more homogeneous silica networks could yield large gains in reduced plate height and separation impedance. Comparing the three-dimensional TSC model with a 2D array of cylinders, it was found that the use of the domain size as the characteristic dimension in the reduced plate height expression is much more appropriate than the use of the skeleton size, hence validating earlier approaches adopted in the literature. (C) 2004 Elsevier B.V. All rights reserved.