Abstract
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.
Highlights
IntroductionMethyl acetate (MA) finds extensive use as a solvent, in pharmaceutical and dye industries, and is applied for the manufacture of acetic anhydride (alkylation reagent) as well as for production of bio-ethanol (gasoline additive or fuel substitute) [1,2]
Methyl acetate (MA) finds extensive use as a solvent, in pharmaceutical and dye industries, and is applied for the manufacture of acetic anhydride as well as for production of bio-ethanol [1,2]
Here we report the results obtained from dimethyl ether (DME) carbonylation with Cu-MOR catalysts with different copper loadings and the influence of recrystallization to modify the pore structure of MOR and Cu-MOR
Summary
Methyl acetate (MA) finds extensive use as a solvent, in pharmaceutical and dye industries, and is applied for the manufacture of acetic anhydride (alkylation reagent) as well as for production of bio-ethanol (gasoline additive or fuel substitute) [1,2]. MA production typically involves carbonylation of methanol with CO to form acetic acid followed by esterification using halides and expensive Rh-complex catalysts in a liquid, homogeneous process [3]. Two-stage gas-phase MA production route was recently devised wherein dimethyl ether (DME), which can be formed efficiently and selectively from petro- or biomass-derived syngas via methanol, are carbonylated with CO using solid acid catalysts [4,5,6]. An important challenge that needs to be addressed before this method potentially can find an industrial application is to increase the activity and stability of the solid catalyst for the DME carbonylation
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