DFT study of furfural conversion on a Re/Pt bimetallic surface; Synergetic effect on the promotion of hydrodeoxygenation

He Dong, Ying Zheng*, P. Hu

*Corresponding author for this work

Research output: Contribution to journalArticle

Abstract

Density functional theory (DFT) calculations of furfural conversion were performed via hydrogenation and hydrodeoxygenation pathways on a bimetallic surface, namely, a thin oxygen-covered Re film on Pt(111). In the most stable adsorption conformation, the furyl ring component adsorbs on the Re edge site and the carbonyl oxygen also plays an important role in the adsorption strength. It was found that, while furfural conversion is kinetically favoured in the hydrogenation route to generate furfuryl alcohol, the hydrodeoxygenation mechanism to generate 2-methylfuran and water is thermodynamically favoured. Our results show that the hydrodeoxygenation product 2-methylfuran is achievable via the hydrogenation of furfural into hydroxyalkyl species, followed by C-OH bond cleavage, and successive hydrogenations of the furyl-CH intermediate. However, the production of 2-methylfuran is prohibited as the oxidised Re surface cannot accept further oxygen deposition, due to the oxygen-related species are difficult to remove in the form of water via hydrogenation. By comparing the results from the Re/Pt system to those on a monometallic flat Pt surface, we were able to demonstrate that incorporation of the oxophilic metals to active metals for hydrogenation could promote the hydrodeoxygenation route by reducing the barrier of C-O bond cleavage.

Original languageEnglish
Pages (from-to)8384-8393
Number of pages10
JournalPhysical Chemistry Chemical Physics
Volume21
Issue number16
Early online date22 Mar 2019
DOIs
Publication statusPublished - 28 Apr 2019

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Furaldehyde
promotion
Hydrogenation
hydrogenation
Density functional theory
density functional theory
Oxygen
oxygen
cleavage
Metals
furfuryl alcohol
routes
Adsorption
adsorption
Water
metals
water
Conformations
flat surfaces
methylidyne

Cite this

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title = "DFT study of furfural conversion on a Re/Pt bimetallic surface; Synergetic effect on the promotion of hydrodeoxygenation",
abstract = "Density functional theory (DFT) calculations of furfural conversion were performed via hydrogenation and hydrodeoxygenation pathways on a bimetallic surface, namely, a thin oxygen-covered Re film on Pt(111). In the most stable adsorption conformation, the furyl ring component adsorbs on the Re edge site and the carbonyl oxygen also plays an important role in the adsorption strength. It was found that, while furfural conversion is kinetically favoured in the hydrogenation route to generate furfuryl alcohol, the hydrodeoxygenation mechanism to generate 2-methylfuran and water is thermodynamically favoured. Our results show that the hydrodeoxygenation product 2-methylfuran is achievable via the hydrogenation of furfural into hydroxyalkyl species, followed by C-OH bond cleavage, and successive hydrogenations of the furyl-CH intermediate. However, the production of 2-methylfuran is prohibited as the oxidised Re surface cannot accept further oxygen deposition, due to the oxygen-related species are difficult to remove in the form of water via hydrogenation. By comparing the results from the Re/Pt system to those on a monometallic flat Pt surface, we were able to demonstrate that incorporation of the oxophilic metals to active metals for hydrogenation could promote the hydrodeoxygenation route by reducing the barrier of C-O bond cleavage.",
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DFT study of furfural conversion on a Re/Pt bimetallic surface; Synergetic effect on the promotion of hydrodeoxygenation. / Dong, He; Zheng, Ying; Hu, P.

In: Physical Chemistry Chemical Physics, Vol. 21, No. 16, 28.04.2019, p. 8384-8393.

Research output: Contribution to journalArticle

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