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A DFT study on Zr-SBA-15 catalyzed ethanol to 1, 3-butadiene


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 on the molecular level. To identify the critical reactive intermediates of ethanol catalysis to catalytically form 1, 3-butadiene on Zr-SBA-15 surface, the model of Zr-SBA-15 was built firstly. 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 lower energy barrier than dehydrogenation to yield acetaldehyde, which means they are competing reactive pathways. C-C bond coupling to form acetaldol (3-hydroxybutanal) is preceded with 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 is hardly carried out. The results here provide a first glimpse into the overall 1,3-butadiene formation mechanism on Zr-SBA-15 reactive sites in light of the two discussing variety of the proposed mechanistic pathways mostly based on conventional homogenous organic chemistry reactions.

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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, Accepted Manuscript
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    A DFT study on Zr-SBA-15 catalyzed ethanol to 1, 3-butadiene

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

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