Cascade Reactions in Tunable Lamellar Micro‐ and Mesopores for C=C Bond Coupling and Hydrocarbon Synthesis

Two‐dimensional MFI zeolite nanosheets contain Brønsted acid sites partially confined at the intercept between micro‐ and mesopores. These acid sites exhibit exceptional reactivities and stabilities for C=C bond coupling and ring‐closure reactions that transform light aldehydes to aromatics. These sites are much more effective than those confined within the micropores of MFI crystallites and those unconfined on H4SiW12O40 clusters or mesoporous aluminosilicate Al‐MCM‐41. The partially confined site environment solvates and stabilizes the transition states of the kinetically relevant steps during aromatization. Lamellar MFI zeolite nanosheets (2D‐MFI) contain a large fraction of partially confined H+ sites (H+pc ) residing at the micro‐ and mesopore intercepts, which are effective for C=C bond coupling and ring closure of aldehydes to produce aromatic compounds. These sheets resemble a nanometer‐sized plug flow reactor; they promote formation and effective removal of aromatic products in cascade reactions, thus mitigating coke deposition.