Molecular Regulator in Mordenite-Catalyzed DME Carbonylation: Eliminating Deactivation Sites, Modulating Microenvironments, and Enhancing Activity

Zeolites are commonly used as catalysts for heterogeneous catalytic reactions. However, severe deactivation of zeolite catalysts often occurs during certain reactions. The regulation of zeolite deactivation is a significant challenge in heterogeneous catalyst design. In this study, we present organic molecular regulators, like 2,6-lutidine, to preferentially adsorb at the T4-O24 site of the mordenite (MOR) zeolite, thereby modulating the microenvironment of the reaction and managing catalyst deactivation. The H-site in the MOR can be used as a pothook to link organic molecule regulators to control the reaction. In comparison to general pyridine molecules, this molecular regulator has less effect on the mass transfer of the reactants and intermediate species, simultaneously contributing to a robust CO activation capability. The strategy of this molecular regulator has yielded a remarkable methyl acetate production rate of up to 1.48 mmol gcat–1 h–1 while exhibiting commendable stability. The use of such molecular regulators presents a promising avenue for extending the operational lifespan and effectiveness of zeolite catalysts, thus paving the way for more robust and efficient industrial chemical processes.