Diffusion and reaction within porous media involving condensable vapors are important processes in catalysis, fuel cells, and membrane separations. In this work, 3-D maps of the spatial variation of porosity, pore size and network tortuosity within a porous solid, derived from magnetic resonance images, have been used to construct a structural model for a mesoporous catalyst pellet. Simulations of the kinetic uptake, adsorption and capillary condensation of butane vapor within the porous solid, conducted on the structural model, have successfully predicted experimental measurements of the effects of the onset of capillary condensation on mass transfer rates without the need of the various adjustable parameters prevalent in other models. These findings suggest that accurate mathematical models for both the complex void space of the porous medium, and the mass transport processes taking place within it, have been successfully developed. (c) 2006 American Institute of Chemical Engineers.