An unexpected pathway for the catalytic oxidation of methylidyne on Rh{111} as a route to syngas.

This study investigates the adsorption properties of methylidyne (CH) on Rh{111}, its partial and full oxidation as well as its surface mobility, by means of plane-wave density functional theory (DFT) calculations. Besides investigating known oxidation pathways on rhodium, such as decomposition of C...

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Main Authors: Inderwildi, O, Jenkins, S, King, D
Format: Journal article
Language:English
Published: 2007
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author Inderwildi, O
Jenkins, S
King, D
author_facet Inderwildi, O
Jenkins, S
King, D
author_sort Inderwildi, O
collection OXFORD
description This study investigates the adsorption properties of methylidyne (CH) on Rh{111}, its partial and full oxidation as well as its surface mobility, by means of plane-wave density functional theory (DFT) calculations. Besides investigating known oxidation pathways on rhodium, such as decomposition of CH and subsequent oxidation of the decomposition products, new pathways such as direct reaction of methylidyne and oxygen toward a surface aldyhyde-type species and the decomposition of this species are considered. The unexpected and novel pathway determined here by DFT is utilized for a microkinetic model of the formation of CO and CO2 from methylidyne. A comparison of this microkinetic study with experimental data shows that our novel mechanism can indeed describe the observations. This comparison strongly suggests that this new alternative route is the main reaction pathway for the conversion of methylidyne.
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spelling oxford-uuid:0c8d48d5-4a9d-4e48-be2d-cee04fd53fc22022-03-26T09:35:43ZAn unexpected pathway for the catalytic oxidation of methylidyne on Rh{111} as a route to syngas.Journal articlehttp://purl.org/coar/resource_type/c_dcae04bcuuid:0c8d48d5-4a9d-4e48-be2d-cee04fd53fc2EnglishSymplectic Elements at Oxford2007Inderwildi, OJenkins, SKing, DThis study investigates the adsorption properties of methylidyne (CH) on Rh{111}, its partial and full oxidation as well as its surface mobility, by means of plane-wave density functional theory (DFT) calculations. Besides investigating known oxidation pathways on rhodium, such as decomposition of CH and subsequent oxidation of the decomposition products, new pathways such as direct reaction of methylidyne and oxygen toward a surface aldyhyde-type species and the decomposition of this species are considered. The unexpected and novel pathway determined here by DFT is utilized for a microkinetic model of the formation of CO and CO2 from methylidyne. A comparison of this microkinetic study with experimental data shows that our novel mechanism can indeed describe the observations. This comparison strongly suggests that this new alternative route is the main reaction pathway for the conversion of methylidyne.
spellingShingle Inderwildi, O
Jenkins, S
King, D
An unexpected pathway for the catalytic oxidation of methylidyne on Rh{111} as a route to syngas.
title An unexpected pathway for the catalytic oxidation of methylidyne on Rh{111} as a route to syngas.
title_full An unexpected pathway for the catalytic oxidation of methylidyne on Rh{111} as a route to syngas.
title_fullStr An unexpected pathway for the catalytic oxidation of methylidyne on Rh{111} as a route to syngas.
title_full_unstemmed An unexpected pathway for the catalytic oxidation of methylidyne on Rh{111} as a route to syngas.
title_short An unexpected pathway for the catalytic oxidation of methylidyne on Rh{111} as a route to syngas.
title_sort unexpected pathway for the catalytic oxidation of methylidyne on rh 111 as a route to syngas
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