Frustrated Lewis pairs constructed on Cs‐Beta for aldol condensation of methyl acetate with formaldehyde

Abstract The solid frustrated Lewis pairs (FLPs) catalyst is a new promising field in catalysis but replete with challenges regarding catalyst preparation and characterization. Herein, a facile acid–base reconstruction strategy is proposed for FLPs catalyst construction based on Beta zeolite. Cs + was first induced by the hydrated extra‐framework aluminum (EFAL) Lewis acid site to form unstable acid–base adducts. Then, Cs + migrates to adjacent Si‐OH and develops Si–O–Cs Lewis base species under elevated temperature while regenerating EFAL Lewis acid centers, establishing FLP structure. A spectroscopic method for competitive adsorption of acid–base molecules has been established for characterizing FLPs, and the moderate‐strong strength Lewis acid–base pairs were confirmed on 8.1Cs‐Beta‐ex by systematic characterization. This engineered FLPs catalyst demonstrates exceptional synergy in aldol condensation of methyl acetate and formaldehyde to methyl acrylate, achieving a 5.8‐fold enhancement in STY versus conventional impregnated catalysts at ca. 8 wt% Cs loading.