Weaving Zeolite into Long‐Lived Catalysts

ABSTRACT The spatial distribution of aluminum in zeolites plays a crucial role in optimizing their catalytic performance. Existing strategies often rely on combinations of inorganic and organic structure‐directing agents to guide crystal growth and aluminum incorporation. However, these methods typically result in zeolite crystals with an aluminum‐rich surface, providing limited control over the spatial placement of aluminum within the crystal structure. In this study, we explore an alternative “weaving” strategy aimed at synthesizing zeolites with alternating Al‐rich and Si‐rich nanodomains within single crystals. This approach involves the physical blending of two separately aged, amorphous sols with contrasting Si/Al ratios, followed by freeze‐drying and steam‐assisted crystallization of the resulting solid in vapor. Unlike conventional hydrothermal synthesis, which produces zeolites with Al‐enriched crystal surfaces, this modularized assembly enables systematic modulation of aluminum distribution, resulting in zeolite crystals with comparable bulk and surface Si/Al ratios, an uncommon feature for high‐silica zeolites. The resulting interwoven zeolites, with closely matched bulk and surface Si/Al ratios, exhibit nearly a twofold increase in catalytic lifetime in the methanol‐to‐hydrocarbons reaction compared to a reference zeolite with a similar bulk composition but significant surface aluminum enrichment, underscoring the significant impact of aluminum spatial distribution on catalytic stability.