Issue 9, 2014

Oxidation of methanol to methyl formate over supported Pd nanoparticles: insights into the reaction mechanism at low temperature

Abstract

Pd nanoparticles supported on TiO2 and SiO2 (2 wt.%) were synthesized by the water-in-oil microemulsion method. The materials were characterized by standard physico-chemical methods (XRD, ICP, TEM, BET, XPS) and DRIFT in operando mode and tested in the gas-phase reaction of methanol oxidation. The direct formation of methyl formate (MF) from methanol was observed. Supported palladium catalysts produced methyl formate at low temperature (<100 °C) with high selectivity. At higher temperatures methyl formate is no longer formed and the total oxidation to CO2 occurred. The DRIFT-operando study confirmed that methanol is adsorbed mainly in two forms, the undissociated gaseous methanol (via H bond) and dissociatively adsorbed methoxy species (CH3O) on the surface. Methyl formate is formed already at RT with the maximum at about 80 °C. The mechanism of the formation of methyl formate from methanol at low temperature is discussed.

Graphical abstract: Oxidation of methanol to methyl formate over supported Pd nanoparticles: insights into the reaction mechanism at low temperature

Article information

Article type
Paper
Submitted
24 Apr 2014
Accepted
07 Jun 2014
First published
09 Jun 2014

Catal. Sci. Technol., 2014,4, 3298-3305

Author version available

Oxidation of methanol to methyl formate over supported Pd nanoparticles: insights into the reaction mechanism at low temperature

R. Wojcieszak, A. Karelovic, E. M. Gaigneaux and P. Ruiz, Catal. Sci. Technol., 2014, 4, 3298 DOI: 10.1039/C4CY00531G

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