A computational study of adsorption and activation of CO2 and H2 over Fe(100) surface

Haozhi Wang, Xiaowa Nie, Xinwen Guo, Chunshan Song

Research output: Contribution to journalArticle

10 Citations (Scopus)

Abstract

Graphical abstract: Periodic density functional theory calculations were performed to investigate the adsorption and activation of CO2 and H2 over Fe(100) surface. Four stable adsorption configurations of CO2 were identified and the energetically most stable adsorption was found to occur on the 4-fold hollow site where the C atom of CO2 sits right above the second layer Fe atom and the two O atoms bound at the center of two FeFe bridge bonds on the surface. H2 molecule dissociates to H* atoms upon adsorption. Only when H2 adsorbs on the top sites of the metal surface it can be stabilized in an associative or molecular form. Small energy barriers were found for H2 dissociation on Fe(100) which indicates that H2 dissociates very fast on the catalyst surface. CO2 adsorption stability could be influenced by the surface coverage of H*. We observed a significant decrease of CO2 adsorption strength when surface H* coverage becomes higher than 2/3 ML.

Original languageEnglish (US)
Pages (from-to)107-114
Number of pages8
JournalJournal of CO2 Utilization
Volume15
DOIs
StatePublished - Sep 1 2016

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Chemical activation
adsorption
Adsorption
Atoms
Energy barriers
Density functional theory
Metals
catalyst
fold
Catalysts
Molecules
metal
energy

All Science Journal Classification (ASJC) codes

  • Chemical Engineering (miscellaneous)
  • Waste Management and Disposal
  • Process Chemistry and Technology

Cite this

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abstract = "Graphical abstract: Periodic density functional theory calculations were performed to investigate the adsorption and activation of CO2 and H2 over Fe(100) surface. Four stable adsorption configurations of CO2 were identified and the energetically most stable adsorption was found to occur on the 4-fold hollow site where the C atom of CO2 sits right above the second layer Fe atom and the two O atoms bound at the center of two FeFe bridge bonds on the surface. H2 molecule dissociates to H* atoms upon adsorption. Only when H2 adsorbs on the top sites of the metal surface it can be stabilized in an associative or molecular form. Small energy barriers were found for H2 dissociation on Fe(100) which indicates that H2 dissociates very fast on the catalyst surface. CO2 adsorption stability could be influenced by the surface coverage of H*. We observed a significant decrease of CO2 adsorption strength when surface H* coverage becomes higher than 2/3 ML.",
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A computational study of adsorption and activation of CO2 and H2 over Fe(100) surface. / Wang, Haozhi; Nie, Xiaowa; Guo, Xinwen; Song, Chunshan.

In: Journal of CO2 Utilization, Vol. 15, 01.09.2016, p. 107-114.

Research output: Contribution to journalArticle

TY - JOUR

T1 - A computational study of adsorption and activation of CO2 and H2 over Fe(100) surface

AU - Wang, Haozhi

AU - Nie, Xiaowa

AU - Guo, Xinwen

AU - Song, Chunshan

PY - 2016/9/1

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N2 - Graphical abstract: Periodic density functional theory calculations were performed to investigate the adsorption and activation of CO2 and H2 over Fe(100) surface. Four stable adsorption configurations of CO2 were identified and the energetically most stable adsorption was found to occur on the 4-fold hollow site where the C atom of CO2 sits right above the second layer Fe atom and the two O atoms bound at the center of two FeFe bridge bonds on the surface. H2 molecule dissociates to H* atoms upon adsorption. Only when H2 adsorbs on the top sites of the metal surface it can be stabilized in an associative or molecular form. Small energy barriers were found for H2 dissociation on Fe(100) which indicates that H2 dissociates very fast on the catalyst surface. CO2 adsorption stability could be influenced by the surface coverage of H*. We observed a significant decrease of CO2 adsorption strength when surface H* coverage becomes higher than 2/3 ML.

AB - Graphical abstract: Periodic density functional theory calculations were performed to investigate the adsorption and activation of CO2 and H2 over Fe(100) surface. Four stable adsorption configurations of CO2 were identified and the energetically most stable adsorption was found to occur on the 4-fold hollow site where the C atom of CO2 sits right above the second layer Fe atom and the two O atoms bound at the center of two FeFe bridge bonds on the surface. H2 molecule dissociates to H* atoms upon adsorption. Only when H2 adsorbs on the top sites of the metal surface it can be stabilized in an associative or molecular form. Small energy barriers were found for H2 dissociation on Fe(100) which indicates that H2 dissociates very fast on the catalyst surface. CO2 adsorption stability could be influenced by the surface coverage of H*. We observed a significant decrease of CO2 adsorption strength when surface H* coverage becomes higher than 2/3 ML.

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