Journal
JOURNAL OF CATALYSIS
Volume 399, Issue -, Pages 132-141Publisher
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcat.2021.04.029
Keywords
C2+ oxygenates; Mordenite; Carbonylation; Ethanol; Acetic acid; Syngas
Categories
Funding
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division, Catalysis Science Program
- National Science Foundation [ECCS-1542152]
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Selective and stable production of C-2 oxygenates from syngas is achieved by using a phosphate-passivated mordenite catalyst in tandem with a commercial Cu/ZnO/AlMgOx catalyst. The phosphate groups cap aluminum sites in mordenite to reduce Bronsted acidity, resulting in over 96% C-2 oxygenate selectivity. This novel catalyst system shows promising potential in syngas conversion processes.
Selective and stable production of C-2 oxygenates from syngas is enabled by a phosphate-passivated mordenite catalyst used in tandem with a commercial Cu/ZnO/AlMgOx catalyst. Unmodified mordenite used in this arrangement is accompanied by substantial hydrocarbon formation and carbon deposition. Therefore, phosphate groups are used to remove or significantly reduce Bronsted acidity in mordenite by capping aluminum sites. Such groups are stable to calcination and catalyst regeneration. Trimethylphosphite is used as a phosphate precursor because it is able to enter the 12 membered-ring pores of mordenite where hydrocarbon formation occurs, but not enter the 8 membered-ring side pockets, where methanol carbonylation occurs selectively. The catalyst was characterized using X-ray fluorescence, X-ray diffraction, and thermal gravimetric analysis. Optionally, a third bed of Cu/ZnO/AlMgOx catalyst is able to hydrodeoxygenate acetic acid to ethanol. The C-2 oxygenate selectivity is over 96% and among the best reported in a single reactor with a syngas feed. (C) 2021 Published by Elsevier Inc.
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