Integrated Stefan-Maxwell, Mean Field, and Single-Event Microkinetic Methodology for Simultaneous Diffusion and Reaction inside Microporous Materials

The assessment of intrinsic reaction kinetics in the presence of diffusion limitations within a porous material remains one of the key challenges within the field of catalysis. The model-guided design of medium-pore zeolite catalysts which typically give rise to mass transport limitations would offer a feasible alternative to conventional trial-and-error procedures. Intracrystalline diffusion limitations during n-hexane hydroconversion on Pt/H-ZSM5 were assessed using an integrated Stefan−Maxwell, mean field, and Single-Event MicroKinetic (SEMK) methodology. The former theory quantifies multicomponent diffusion through a microporous substituent from pure component properties, while framework parameters inherent to the ZSM5 topology are incorporated via a mean field approximation. The complex chemistry involved in n-hexane hydroconversion was described by an SEMK model which is based upon the reaction family concept. Model regression against experimental data resulted in excellent agreement between the model and experiment. In addition, the estimated values for, among others, the component diffusion coefficients were physically meaningful. A sensitivity analysis of the catalyst descriptors demonstrated that especially the total acid site concentration and the crystallite geometry impact the catalyst activity and product distribution, establishing them as critical catalyst design parameters.status: publishe