Loading-Driven Diffusion Pathway Selectivity in Zeolites with Continuum Intersecting Channels

Abstract

The diffusion processes in zeolites are important for heterogeneous catalysis. Herein, we show that unique zeolites with "continuum intersecting channels" (e.g., BEC, POS, and SOV), in which two intersections are proximal, are greatly significant to the diffusion process with spontaneous switching of the diffusion pathway under varied loading. At low loading, the synergy of strong adsorption sites and molecular reorientation in intersections contribute to almost exclusive molecular diffusion in smaller channels. With an increase in molecular loading, the adsorbates are transported preferentially in larger channels mainly due to the lower diffusion barrier inside continuum intersection channels. This work demonstrates the ability to adjust the prior diffusion pathway by controlling the molecular loading, which may be beneficial for the separation of the product and byproduct in heterogeneous catalysis.