Theoretical and numerical investigations of TAP experiments: new approaches for variable pressure conditions

Abstract

Temporal analysis of products (“TAP”, see Gleaves et al. in Catal Rev Sci Eng 30:49, 1988) is a valuable tool for characterisation of porous catalytic structures. Established TAP-modelling requires a spatially constant diffusion coefficient and neglect convective flows, which is only valid in Knudsen diffusion regime. A new theoretical model is developed for estimating the number of molecules per pulse to stay in Knudsen diffusion regime under any conditions and at any time. Moreover a new methodology for generating a full three-dimensional geometrical representation of beds is presented and used for numerical simulations. In computational fluid dynamics software (ANSYS CFX® version 14) a transient diffusive transport equation with time-dependent inlet boundary conditions is solved. Three different pellet diameters were investigated with 1E+18 molecules per pulse, which is higher than the limit from the theoretical calculation (about 1E+15). From this results, the distance from inlet can be calculated where the theoretical pressure limit (Kn = 2) is obtained, i.e., from this point to the end of reactor, Knudsen regime can be assumed.