Journal
JOURNAL OF CATALYSIS
Volume 269, Issue 1, Pages 44-52Publisher
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcat.2009.10.014
Keywords
Methanol carboxylation; Dimethyl carbonate; Effect of Al2O3 on CeO2 catalysts; Surface modification; Surface techniques; DRIFT studies; NMR solid state and solution; Reaction mechanism
Categories
Funding
- EU-IP TOPCOMBI
- Hungarian Research Foundation (OTKA) [K-60549]
- University of Bari
- MiUR
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In this paper we show that modification of ceria by loading alumina strongly reduces the oxidation of methanol and the consequent reduction of Ce(IV) to Ce(III) with increase of both the life of the catalysts and their selectivity. The combination of surface techniques (XPS and BET) with structural techniques (XRD) has allowed a good characterisation of the working catalysts. Spectroscopic analyses (DRIFT) and multinuclear solid state and solution NMR) have permitted the monitoring of the species formed on the surface of the catalyst and released from it. The formation of DMC takes place in successive steps such as (i) interaction of methanol with the catalyst surface with the formation of the surface-bound -OCH3; (ii) building on the catalyst surface of the hemicarbonate moiety [-OCH3 -> -OC(C)OCH3]; and (iii) reaction of the latter with the gas-phase methanol to afford the organic carbonate. (c) 2009 Elsevier Inc. All rights reserved.
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