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

Valerie Eta; Päivi Mäki-Arvela; Johan Wärnå; Tapio Salmi; Jyri-Pekka Mikkola; Dmitry Yu Murzin

doi:10.1016/j.apcata.2011.07.004

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

Valerie Eta, Päivi Mäki-Arvela, Johan Wärnå, Tapio Salmi, Jyri-Pekka Mikkola, Dmitry Yu Murzin^*

^*Corresponding author for this work

Laboratory of Industrial Chemistry and Reaction Engineering

Research output: Contribution to journal › Article › Scientific › peer-review

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Abstract

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.

Original language	English
Pages (from-to)	39-46
Number of pages	8
Journal	Applied Catalysis A: General
Volume	404
Issue number	1-2
DOIs	https://doi.org/10.1016/j.apcata.2011.07.004
Publication status	Published - 19 Sept 2011
MoE publication type	A1 Journal article-refereed

Keywords

Butylene oxide
Carbon dioxide
Dimethyl carbonate
Kinetics
Methanol
ZrO -MgO

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

abstract = "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.",

keywords = "Butylene oxide, Carbon dioxide, Dimethyl carbonate, Kinetics, Methanol, ZrO -MgO",

author = "Valerie Eta and P{\"a}ivi M{\"a}ki-Arvela and Johan W{\"a}rn{\aa} and Tapio Salmi and Jyri-Pekka Mikkola and Murzin, {Dmitry Yu}",

note = "Funding Information: This work is part of the activities of {\AA}bo Akademi Process Chemistry Centre within the Finnish Centre of Excellence (2006–2011), and the KETJU Research Programme (2006–2010) by the Academy of Finland. The authors are grateful to the Academy of Finland for the financial support under the Grants 120853, 124357 and 128626. This work is also associated with the activities of Ume{\aa} University Chemical-Biological Centre whereupon financial support from Bio4Energy Programme, Kempe Foundations and Knut and Alice Wallenberg Foundation are acknowledged. Copyright: Copyright 2011 Elsevier B.V., All rights reserved.",

year = "2011",

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day = "19",

doi = "10.1016/j.apcata.2011.07.004",

language = "English",

volume = "404",

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AU - Eta, Valerie

AU - Mäki-Arvela, Päivi

AU - Wärnå, Johan

AU - Salmi, Tapio

AU - Mikkola, Jyri-Pekka

AU - Murzin, Dmitry Yu

N1 - Funding Information: This work is part of the activities of Åbo Akademi Process Chemistry Centre within the Finnish Centre of Excellence (2006–2011), and the KETJU Research Programme (2006–2010) by the Academy of Finland. The authors are grateful to the Academy of Finland for the financial support under the Grants 120853, 124357 and 128626. This work is also associated with the activities of Umeå University Chemical-Biological Centre whereupon financial support from Bio4Energy Programme, Kempe Foundations and Knut and Alice Wallenberg Foundation are acknowledged. Copyright: Copyright 2011 Elsevier B.V., All rights reserved.

PY - 2011/9/19

Y1 - 2011/9/19

N2 - 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.

AB - 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.

KW - Butylene oxide

KW - Carbon dioxide

KW - Dimethyl carbonate

KW - Kinetics

KW - Methanol

KW - ZrO -MgO

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VL - 404

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ER -

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

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Keywords

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