Diffusion is an extremely critical step in zeolite catalysis that determines the catalytic performance, in particular for the conversion of bulky molecules. Introducing interconnected mesopores and macropores into a single microporous zeolite with the rationalized pore size at each level is an effective strategy to suppress the diffusion limitations, but remains highly challenging due to the lack of rational design principles. Herein, we demonstrate the first example of boosting molecular diffusion by constructing hierarchical Murray zeolites with a highly ordered and fully interconnected macro-meso-microporous structure on the basis of the generalized Murray's Law. Such a hierarchical Murray zeolite with a refined quantitative relationship between the pore size at each length scale exhibited 9 and 5 times higher effective diffusion rates, leading to 2.5 and 1.5 times higher catalytic performance in the bulky 1,3,5-triisopropylbenzene cracking reaction than those of microporous ZSM-5 and ZSM-5 nanocrystals, respectively. The concept of hierarchical Murray zeolites with optimized structural features and their design principles could be applied to other catalytic reactions for maximized performance.
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