Reaction rate enhancement in nanoporous materials with single-file behaviour

In the concept of "molecular traffic control", Derouane and Gabelica postul ated an enhancement of the effective conversion rate in catalytic reactions if the reactant and product molecules avoid each other by preferentially c hoosing different channel systems on their diffusion path into and out of t he catalyst particles. After two decades of controversial discussions, the feasibility of this concept has recently been demonstrated by considering a network of intersecting single-tile channels, whose accessibility by the r eactant and product molecules was mutually excluded. The present communicat ion analyses the dependence of molecular distribution over the different el ements of the channel system on the intrinsic reactivity and the pore filli ng factor. The obtained patterns are compared with those of a reference sys tem where all channels are equally accessible by the reactant and product m olecules. Special attention is given to the effect of particle self-blockag es under molecular traffic control, which occurs for large intrinsic reacti vities and pore filling factors. It is demonstrated that under these condit ions the simulations end up in an immobilised state which is a function of the particular simulation run. Such a behaviour is not observable in the re ference system.