Dimethyl carbonate synthesis from carbon dioxide and methanol over CeO2 versus over ZrO2: comparison of mechanisms

Lei Chen; Shengping Wang; Jingjie Zhou; Yongli Shen; Yujun Zhao; Xinbin Ma

doi:10.1039/C4RA03081H

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Dimethyl carbonate synthesis from carbon dioxide and methanol over CeO₂versus over ZrO₂: comparison of mechanisms

Lei Chen,^a Shengping Wang,*^a Jingjie Zhou,^a Yongli Shen,^a Yujun Zhao^a and Xinbin Ma^a

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* Corresponding authors

^a Key Laboratory for Green Chemical Technology, School of Chemical Engineering and Technology, Tianjin University, Collaborative Innovation Center of Chemical Science and Engineering, Tianjin 300072, China
E-mail: spwang@tju.edu.cn
Fax: +86-22-87401818
Tel: +86-22-87401818

Abstract

A comparison of the mechanisms of dimethyl carbonate (DMC) formation directly from carbon dioxide and methanol over CeO₂ versus over ZrO₂ is made through in situ Fourier transform infrared spectroscopy (FTIR). During the reaction involving methanol and CO₂ adsorption over CeO₂, a new band appears at around 1295 cm⁻¹. Combining this result with in situ FTIR results of methyl formate adsorption, this band is assigned to carbomethoxide, which is taken as the intermediate in DMC formation over the ceria surface. Carbomethoxide originates from the reaction of methanol and adsorbed carbon dioxide; its formation is followed by reaction with a methoxy group to form DMC. This mechanism differs from that occurring on zirconium oxide, in which DMC is formed by the reaction between monodentate methyl carbonate and methanol.

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DOI: https://doi.org/10.1039/C4RA03081H
Article type: Paper
Submitted: 07 Apr 2014
Accepted: 18 Jun 2014
First published: 19 Jun 2014

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RSC Adv., 2014,4, 30968-30975

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Dimethyl carbonate synthesis from carbon dioxide and methanol over CeO₂ versus over ZrO₂: comparison of mechanisms

L. Chen, S. Wang, J. Zhou, Y. Shen, Y. Zhao and X. Ma, RSC Adv., 2014, 4, 30968 DOI: 10.1039/C4RA03081H

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