The mechanism of CO2 chemisorption on zigzag carbon active sites: A computational chemistry study

Research output: Contribution to journalArticle

59 Citations (Scopus)

Abstract

A computational chemistry study was carried out to evaluate the various options for CO2 adsorption on one or two adjacent zigzag sites in a graphene layer. Density functional theory was used with the 6-31G(d) basis set, as implemented in the Gaussian software package in conjunction with GaussView and Chem3D. Various electronic environments of a four-ring model, with and without surface oxygen and with special emphasis on carbene-like structures, were analyzed. The resulting optimized geometries were quite sensitive to such electronic configurations. In agreement with long-standing experimental evidence, dissociative CO2 adsorption was found to be particularly favorable; furthermore, dissociation was found to be favored on isolated carbene-like zigzag sites. It is recommended that such a pathway, rather than dual-site adsorption and C-CO2 complex formation, deserves the dominant attention in further theoretical studies of adsorption, reaction and desorption processes during CO2 gasification of carbons.

Original languageEnglish (US)
Pages (from-to)907-915
Number of pages9
JournalCarbon
Volume43
Issue number5
DOIs
StatePublished - Mar 4 2005

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Computational chemistry
Chemisorption
Carbon
Adsorption
Graphite
Gasification
Software packages
Graphene
Density functional theory
Desorption
Oxygen
Geometry
carbene

All Science Journal Classification (ASJC) codes

  • Chemistry(all)
  • Materials Science(all)

Cite this

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abstract = "A computational chemistry study was carried out to evaluate the various options for CO2 adsorption on one or two adjacent zigzag sites in a graphene layer. Density functional theory was used with the 6-31G(d) basis set, as implemented in the Gaussian software package in conjunction with GaussView and Chem3D. Various electronic environments of a four-ring model, with and without surface oxygen and with special emphasis on carbene-like structures, were analyzed. The resulting optimized geometries were quite sensitive to such electronic configurations. In agreement with long-standing experimental evidence, dissociative CO2 adsorption was found to be particularly favorable; furthermore, dissociation was found to be favored on isolated carbene-like zigzag sites. It is recommended that such a pathway, rather than dual-site adsorption and C-CO2 complex formation, deserves the dominant attention in further theoretical studies of adsorption, reaction and desorption processes during CO2 gasification of carbons.",
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The mechanism of CO2 chemisorption on zigzag carbon active sites : A computational chemistry study. / Radovic, Ljubisa R.

In: Carbon, Vol. 43, No. 5, 04.03.2005, p. 907-915.

Research output: Contribution to journalArticle

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