An experimental and theoretical study of dimethyl carbonate synthesis on cu-y zeolite

FUEL 90

A. T. Bell, bell@cchem.berkeley.edu, Department of Chemical Engineering, University of California, Berkeley, CA 94720-1462
Experimental and theoretical studies were carried out to define the mechanism and kinetics of the oxidative carbonylation of methanol to dimethyl carbonate (DMC) on Cu-Y. Cu is exchanged into H-Y zeolite by high-temperature reaction with CuCl vapor. Brønsted acid protons are completely exchanged by Cu+, as confirmed by IR spectroscopy, XANES and EXAFS. Upon contact with CH3OH and O2, mono-and di-methoxide species bound to Cu+ cations are formed rapidly. The rate-limiting step in DMC formation is the reaction of CO with mono-methoxide species to form mono-methyl carbonate species, which then react rapidly with methanol to form DMC. An alternate route is the addition of CO to di-methoxide species to form DMC directly. The reaction mechanism, the rate of DMC formation, and the associated activation energy predicted theoretically are in very good agreement with experiment.
 

Green Chemistry for Sustainable Energy Supply and Conversion
1:45 PM-4:55 PM, Monday, April 7, 2008 Morial Convention Center -- Rm. 242, Oral

Division of Fuel Chemistry

The 235th ACS National Meeting, New Orleans, LA, April 6-10, 2008