Replacing homogeneous catalytic processes by heterogeneous routes based on the utilization of solid catalysts is of great interest from an environmental point of view. Owing to their genuine pore structure, zeolites such as mordenites (MOR) have emerged as game-changing materials to enable the heterogenization of catalytic processes including methanol carbonylation. Cu-exchange zeolites take the edge over pristine zeolites, leading to enhanced catalytic performance in terms of greater activity, selectivity, and stability. Herein, the overall catalytic activity and stability can be modulated upon controlling the environment and location of copper active sites in zeolites. In this study, Cu-exchanged mordenites were strategically synthesized to investigate the role of Cu location inside of MOR cavities under working conditions by means of in situ/operando infrared (IR) spectroscopic studies. The results obtained revealed that a major proportion of Cu in the MR-8 cavities notably enhances the activity and stability of the catalyst. This study provides crucial insights for fine-tuning zeolite catalysts to achieve the heterogenization of homogeneous carbonylation processes.

Financial support for this work has been obtained from the Spanish Ministerio de Ciencia e Innovación through the project SMART-FTS (PID2021-126876OB-I00) sponsored by MCIN/AEI/10.13039/501100011033 and European Union ERDF. Ligia A. Luque Álvarez thanks VI-PPITUS (University of Sevilla) for her current predoctoral contract.

Peer reviewed