Promoting Effect of Copper Loading and Mesoporosity on Cu-MOR in the Carbonylation of Dimethyl Ether to Methyl Acetate

• Main Authors: Raju Poreddy, Susanne Mossin, Anker Degn Jensen, Anders Riisager
• Format: Article
• Language: English
• Published: MDPI AG 2021-05-01
• Series: Catalysts
• Subjects: carbonylation; dimethyl ether; methyl acetate; Cu-Mordenite; recrystallization
• Online Access: https://www.mdpi.com/2073-4344/11/6/696

Cu-mordenite (Cu-MOR) catalysts with different copper loadings were prepared, characterized and examined in continuous, gas-flow synthesis of methyl acetate (MA) by dimethyl ether (DME) carbonylation. Improved activity and selectivity were observed for Cu-MOR catalysts with up to 1 wt% Cu and X-ray photoelectron spectroscopy (XPS), electron paramagnetic resonance (EPR) spectroscopy and temperature-programmed reduction with hydrogen (H₂-TPR) were used to elucidate the state of copper in the catalysts. Moreover, mesoporous MOR catalysts (RHMs) were prepared by mild stepwise recrystallization with X-ray powder diffraction (XRPD) and ammonia temperature-programmed desorption (NH₃-TPD) demonstrating the retained MOR structure and the acid property of the catalysts, respectively. The RHM catalysts showed improved lifetime compared to pristine MOR giving a yield up to 78% MA with 93% selectivity after 5 h on stream (GHSV = 6711 h⁻¹). Under identical reaction conditions, 1 wt% Cu-RHM catalysts had an even higher catalytic activity and durability resulting in a MA yield of 90% with 97% selectivity for 7–8 h of operation as well as a lower coke formation.