Reaction kinetics in zeolites as a random walk problem: Theory versus experiment

We present a continuous time random walk (CTRW) model for the kinetics of pseudo-first-order long-range reactions in zeolites assisted by migration between the adsorption sites. Both Markovian and non-Markovian formulations admit a simple matrix solution in terms of the lattice Green's function. Diffuse-reflectance transient absorption study of triplet anthracene quenching by azulene in NaY zeolite is reported giving a direct visual indication of the long-range reaction between molecules residing in the neighboring cages, reflecting an open structure of the cage network. The Markovian model with unbiased nearest-neighbor CTRW on a diamond lattice of NaY supercages explains the experimental decay data. This practical example demonstrates a general possibility to consistently recover information about intercage transport in zeolites and related microporous materials by using an indicator reaction and an appropriate theoretical interpretation, complementary to conventional NMR techniques. (C) 2000 American Institute of Physics. [S0021-9606(00)70131-0].