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Issue 18, 2018
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A DFT study on Zr-SBA-15 catalyzed conversion of ethanol to 1,3-butadiene

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Abstract

Density functional theory (DFT) calculations have been used to elucidate the influence of the surface properties of Zr-SBA-15 on the conversion of ethanol to 1,3-butadiene at the molecular level. To identify the critical reactive intermediates of ethanol catalysis to catalytically form 1,3-butadiene on the Zr-SBA-15 surface, the model of Zr-SBA-15 was first built. The overall enthalpy energy surface was explored for the highly-debated reaction mechanisms, including Toussaint's aldol condensation mechanism and Fripiat's Prins mechanism. It was found that ethanol dehydration to form ethylene possessed a lower energy barrier than dehydrogenation to yield acetaldehyde, which means they are competing reactive pathways. C–C bond coupling to form acetaldol (3-hydroxybutanal) proceeds with a 2.15 eV forward reaction barrier. Direct reaction of ethylene and acetaldehyde proceeds with a free energy barrier of 2.90 eV suggesting that Prins condensation hardly occurs. The results here provide a first glimpse into the overall mechanism of 1,3-butadiene formation on Zr-SBA-15 reactive sites in light of the variety of proposed mechanistic pathways mostly based on conventional homogenous organic chemistry reactions.

Graphical abstract: A DFT study on Zr-SBA-15 catalyzed conversion of ethanol to 1,3-butadiene

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Publication details

The article was received on 25 Dec 2017, accepted on 06 Apr 2018 and first published on 09 Apr 2018


Article type: Paper
DOI: 10.1039/C7CP08620B
Citation: Phys. Chem. Chem. Phys., 2018,20, 12970-12978
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    A DFT study on Zr-SBA-15 catalyzed conversion of ethanol to 1,3-butadiene

    X. Dong, J. Lu, Y. Yu and M. Zhang, Phys. Chem. Chem. Phys., 2018, 20, 12970
    DOI: 10.1039/C7CP08620B

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