Probing the Design Rationale of a High‐Performing Faujasitic Zeotype Engineered to have Hierarchical Porosity and Moderated Acidity

Porosity and acidity are influential properties in the rational design of solid‐acid catalysts. Probing the physicochemical characteristics of an acidic zeotype framework at the molecular level can provide valuable insights in understanding intrinsic reaction pathways, for affording structure–activity relationships. Herein, we employ a variety of probe‐based techniques (including positron annihilation lifetime spectroscopy (PALS), FTIR and solid‐state NMR spectroscopy) to demonstrate how a hierarchical design strategy for a faujasitic (FAU) zeotype (synthesized for the first time, via a soft‐templating approach, with high phase‐purity) can be used to simultaneously modify the porosity and modulate the acidity for an industrially significant catalytic process (Beckmann rearrangement). Detailed characterization of hierarchically porous (HP) SAPO‐37 reveals enhanced mass‐transport characteristics and moderated acidity, which leads to superior catalytic performance and increased resistance to deactivation by coking, compared to its microporous counterpart, further vindicating the interplay between porosity and moderated acidity.