Promoting effect of copper loading and mesoporosity on Cu-MOR in the carbonylation of dimethyl ether to methyl acetate

Raju Poreddy, Susanne Mossin, Anker Degn Jensen, Anders Riisager*

*Corresponding author for this work

Research output: Contribution to journalJournal articleResearchpeer-review

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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.

Original languageEnglish
Article number696
JournalCatalysts
Volume11
Issue number6
ISSN2073-4344
DOIs
Publication statusPublished - 2021

Bibliographical note

Funding Information:
Funding: This research was funded by the UNIK research initiative Catalysis for Sustainable Energy funded by the Danish Ministry of Science, Technology and Innovation.

Publisher Copyright:
© 2021 by the authors. Licensee MDPI, Basel, Switzerland.

Keywords

  • Carbonylation
  • Cu-Mordenite
  • Dimethyl ether
  • Methyl acetate
  • Recrystallization

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