Nature‐Inspired, Computer‐Assisted Optimization of Hierarchically Structured Zeolites

Abstract Zeolite catalysis is often affected by transport limitations, which significantly influence overall performance. Introducing wide pores as molecular transport highways can reduce transport limitations, control the product distribution, and mitigate effects of catalyst deactivation. Nevertheless, the importance to rationally design the meso‐ and macropore space remains underappreciated. This article reviews multiscale modelling approaches to optimize overall catalytic performance. It provides a general methodology and rules of thumb to guide catalyst synthesis with optimal pore network characteristics. Inspiration is taken from nature, such as the structure of leaves and tissues, with similar requirements and associated features. In optimal hierarchically structured zeolites, the added macro‐/mesopore volume fraction, connectivity, crystal size, and minimum wide pore size are crucial. The broad pore size distribution is secondary. No uncontrolled diffusion limitations should exist within the zeolite crystals. Surface barriers, however, can significantly affect, even dominate overall transport. Understanding their origin and ways to control them is an emergent research area. Synthesis methods to realize hierarchically structured zeolites are briefly reviewed. Significant gaps exist between laboratory synthesis methods and industrial requirements. Zeolite catalysis could benefit from computer‐assisted design of their hierarchical pore network, embracing principles used by natural transport networks for scalable efficiency, selectivity, and robustness.