Using DFT in search for support effects during methanol oxidation on supported molybdenum oxides

Tim Fievez; Paul Geerlings; Bert M. Weckhuysen; Frank De Proft

doi:10.1002/cphc.201100607

Using DFT in search for support effects during methanol oxidation on supported molybdenum oxides

Tim Fievez^*, Paul Geerlings, Bert M. Weckhuysen, Frank De Proft

^*Corresponding author for this work

Sub Inorganic Chemistry and Catalysis

Vrije Universiteit Brussel

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

Abstract

The oxidation of methanol on supported molybdenum oxides was studied using DFT. Starting from a cluster model for a mono-oxo and di-oxo molybdenum oxide on a SiO₂ support, the reaction energies and rates for the oxidation of methanol were computed and interpreted with chemical reaction indices. This pointed out that the apparent barrier was significantly lower on the mono-oxide model, favoring it over the di-oxo species. Accordingly, we assumed similar behavior on Al₂O₃, TiO₂ and ZrO₂ supports, so that we could compare characteristics over different supports. The obtained reaction energies and rates followed the experimental turn-over frequency (TOF) sequence.

Original language	English
Pages (from-to)	3281-3290
Number of pages	10
Journal	ChemPhysChem
Volume	12
Issue number	17
DOIs	https://doi.org/10.1002/cphc.201100607
Publication status	Published - 9 Dec 2011

Keywords

density functional theory
electronic structure
molybdenum oxides
supported catalysis
surfaces

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10.1002/cphc.201100607

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abstract = "The oxidation of methanol on supported molybdenum oxides was studied using DFT. Starting from a cluster model for a mono-oxo and di-oxo molybdenum oxide on a SiO2 support, the reaction energies and rates for the oxidation of methanol were computed and interpreted with chemical reaction indices. This pointed out that the apparent barrier was significantly lower on the mono-oxide model, favoring it over the di-oxo species. Accordingly, we assumed similar behavior on Al2O3, TiO2 and ZrO2 supports, so that we could compare characteristics over different supports. The obtained reaction energies and rates followed the experimental turn-over frequency (TOF) sequence.",

keywords = "density functional theory, electronic structure, molybdenum oxides, supported catalysis, surfaces",

author = "Tim Fievez and Paul Geerlings and Weckhuysen, {Bert M.} and {De Proft}, Frank",

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AU - Weckhuysen, Bert M.

AU - De Proft, Frank

PY - 2011/12/9

Y1 - 2011/12/9

N2 - The oxidation of methanol on supported molybdenum oxides was studied using DFT. Starting from a cluster model for a mono-oxo and di-oxo molybdenum oxide on a SiO2 support, the reaction energies and rates for the oxidation of methanol were computed and interpreted with chemical reaction indices. This pointed out that the apparent barrier was significantly lower on the mono-oxide model, favoring it over the di-oxo species. Accordingly, we assumed similar behavior on Al2O3, TiO2 and ZrO2 supports, so that we could compare characteristics over different supports. The obtained reaction energies and rates followed the experimental turn-over frequency (TOF) sequence.

AB - The oxidation of methanol on supported molybdenum oxides was studied using DFT. Starting from a cluster model for a mono-oxo and di-oxo molybdenum oxide on a SiO2 support, the reaction energies and rates for the oxidation of methanol were computed and interpreted with chemical reaction indices. This pointed out that the apparent barrier was significantly lower on the mono-oxide model, favoring it over the di-oxo species. Accordingly, we assumed similar behavior on Al2O3, TiO2 and ZrO2 supports, so that we could compare characteristics over different supports. The obtained reaction energies and rates followed the experimental turn-over frequency (TOF) sequence.

KW - density functional theory

KW - electronic structure

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KW - supported catalysis

KW - surfaces

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Using DFT in search for support effects during methanol oxidation on supported molybdenum oxides

Abstract

Keywords

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