Kinetics of dimethyl carbonate synthesis from methanol and carbon dioxide over ZrO2-MgO catalyst in the presence of butylene oxide as additive

被引:48
作者
Eta, Valerie [1 ]
Maki-Arvela, Paivi [1 ]
Warna, Johan [1 ]
Salmi, Tapio [1 ]
Mikkola, Jyri-Pekka [1 ,2 ]
Murzin, Dmitry Yu. [1 ]
机构
[1] Abo Akad Univ, Proc Chem Ctr, Lab Ind Chem & React Engn, SF-20500 Turku, Finland
[2] Umea Univ, Dept Chem, Chem Biol Ctr, SE-90187 Umea, Sweden
基金
芬兰科学院;
关键词
Dimethyl carbonate; Methanol; Carbon dioxide; Butylene oxide; Kinetics; ZrO2-MgO; CYCLIC CARBONATES; ACTIVATION; ZIRCONIA; COMPLEXES; CO2; CU;
D O I
10.1016/j.apcata.2011.07.004
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
A kinetic investigation of dimethyl carbonate (DMC) synthesis from methanol and CO2 over ZrO2-MgO was performed by using butylene oxide as a chemical trap for the water formed during the reaction. The effect of the catalyst amount, the stirring speed, the temperature, as well as the amount of butylene oxide on the reaction rate and the selectivity to DMC was studied. The analysis of the reaction pathway suggests that DMC and butylene glycol are formed via the reaction of adsorbed mono-methoxycarbonate intermediate and methoxybutanol or methanol. A kinetic model was developed based on the reaction mechanism and it was in agreement with the experimental data. The apparent activation energy for the formation of DMC was 62 kj/mol. (C) 2011 Elsevier B.V. All rights reserved.
引用
收藏
页码:39 / 46
页数:8
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