The effect of alkoxide ionic liquids on the synthesis of dimethyl carbonate from CO2 and methanol over ZrO2-MgO

Valerie Eta; Päivi Mäki-Arvela; Eero Salminen; Tapio Salmi; Dmitry Yu Murzin; Jyri-Pekka Mikkola

doi:10.1007/s10562-011-0666-3

The effect of alkoxide ionic liquids on the synthesis of dimethyl carbonate from CO₂ and methanol over ZrO₂-MgO

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

^*Korresponderande författare för detta arbete

Forskningsoutput: Tidskriftsbidrag › Artikel › Vetenskaplig › Peer review

53 Citeringar (Scopus)

Sammanfattning

The use of carbon dioxide in the synthesis of chemicals, such as dimethyl carbonate (DMC), constitutes an environmentally attractive alternative to hazardous and toxic reagents. However, the direct synthesis of DMC from methanol and CO₂ is characterized by low yields due to the reaction equilibrium and the thermodynamic limitations (ΔG_298K ⁰ = +26.3 kj/mol). Alkoxide ionic liquids possessing alkylimidazolium and benzalkonium cations were prepared, characterised and tested together with ZrO₂-MgO catalyst for the synthesis of DMC from methanol and CO ₂. By using the novel ionic liquid as additives, ca. 12% conversion of methanol, and 90% selectivity to DMC was obtained at 120 °C and 7.5 MPa. The water abstracting potential of the ionic liquids influenced the conversion of methanol and the selectivity to DMC. The alkoxide ionic liquids were recovered and reused in DMC synthesis without loss in activity and selectivity.

Originalspråk	Engelska
Sidor (från-till)	1254-1261
Antal sidor	8
Tidskrift	Catalysis Letters
Volym	141
DOI	https://doi.org/10.1007/s10562-011-0666-3
Status	Publicerad - 2011
MoE-publikationstyp	A1 Tidskriftsartikel-refererad

Finansiering

Acknowledgments 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.

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title = "The effect of alkoxide ionic liquids on the synthesis of dimethyl carbonate from CO2 and methanol over ZrO2-MgO",

abstract = "The use of carbon dioxide in the synthesis of chemicals, such as dimethyl carbonate (DMC), constitutes an environmentally attractive alternative to hazardous and toxic reagents. However, the direct synthesis of DMC from methanol and CO2 is characterized by low yields due to the reaction equilibrium and the thermodynamic limitations (ΔG298K 0 = +26.3 kj/mol). Alkoxide ionic liquids possessing alkylimidazolium and benzalkonium cations were prepared, characterised and tested together with ZrO2-MgO catalyst for the synthesis of DMC from methanol and CO 2. By using the novel ionic liquid as additives, ca. 12\% conversion of methanol, and 90\% selectivity to DMC was obtained at 120 °C and 7.5 MPa. The water abstracting potential of the ionic liquids influenced the conversion of methanol and the selectivity to DMC. The alkoxide ionic liquids were recovered and reused in DMC synthesis without loss in activity and selectivity.",

keywords = "Alkoxide ionic liquid, Carbon dioxide, Dimethyl carbonate, Methanol, ZrO -MgO",

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

note = "Funding Information: Acknowledgments 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",

doi = "10.1007/s10562-011-0666-3",

language = "English",

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pages = "1254--1261",

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AU - Salmi, Tapio

AU - Murzin, Dmitry Yu

AU - Mikkola, Jyri-Pekka

N1 - Funding Information: Acknowledgments 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

Y1 - 2011

N2 - The use of carbon dioxide in the synthesis of chemicals, such as dimethyl carbonate (DMC), constitutes an environmentally attractive alternative to hazardous and toxic reagents. However, the direct synthesis of DMC from methanol and CO2 is characterized by low yields due to the reaction equilibrium and the thermodynamic limitations (ΔG298K 0 = +26.3 kj/mol). Alkoxide ionic liquids possessing alkylimidazolium and benzalkonium cations were prepared, characterised and tested together with ZrO2-MgO catalyst for the synthesis of DMC from methanol and CO 2. By using the novel ionic liquid as additives, ca. 12% conversion of methanol, and 90% selectivity to DMC was obtained at 120 °C and 7.5 MPa. The water abstracting potential of the ionic liquids influenced the conversion of methanol and the selectivity to DMC. The alkoxide ionic liquids were recovered and reused in DMC synthesis without loss in activity and selectivity.

AB - The use of carbon dioxide in the synthesis of chemicals, such as dimethyl carbonate (DMC), constitutes an environmentally attractive alternative to hazardous and toxic reagents. However, the direct synthesis of DMC from methanol and CO2 is characterized by low yields due to the reaction equilibrium and the thermodynamic limitations (ΔG298K 0 = +26.3 kj/mol). Alkoxide ionic liquids possessing alkylimidazolium and benzalkonium cations were prepared, characterised and tested together with ZrO2-MgO catalyst for the synthesis of DMC from methanol and CO 2. By using the novel ionic liquid as additives, ca. 12% conversion of methanol, and 90% selectivity to DMC was obtained at 120 °C and 7.5 MPa. The water abstracting potential of the ionic liquids influenced the conversion of methanol and the selectivity to DMC. The alkoxide ionic liquids were recovered and reused in DMC synthesis without loss in activity and selectivity.

KW - Alkoxide ionic liquid

KW - Carbon dioxide

KW - Dimethyl carbonate

KW - Methanol

KW - ZrO -MgO

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