Density functional studies of the adsorption and dissociation of CO 2 molecule on Fe(111) surface

Hui Lung Chen; Hsin Tsung Chen; Jia Jen Ho

doi:10.1021/la9021646

Density functional studies of the adsorption and dissociation of CO ₂ molecule on Fe(111) surface

Hui Lung Chen^*, Hsin Tsung Chen, Jia Jen Ho

^*Corresponding author for this work

Department of Chemistry

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

25 Citations (Scopus)

Abstract

Spin-polarized density functional theory calculation was carried out to characterize the adsorption and dissociation of CO₂ molecule on the Fe(111) surface. It was shown that the barriers for the stepwise CO₂ dissociation reaction, CO_2(g) →C_(a) + 2O _(a), are 21.73 kcal/mol (for OC-O bond activation) and 23.87 kcal/mol (for C-O bond activation), and the entire process is 35.73 kcal/mol exothermic. The rate constants for the dissociative adsorption of CO₂ have been predicted with variational RRKM theory, and the predicted rate constants, k _CO2 (in unit of cm³ molecule^-1 s^-1), can be represented by the equations 2.12 x 10^-8T^-0.842 exp(-0.258 kcal mol^-1/RT) at T = 100-1000 K. To gain insights into high catalytic activity of the Fe(111) surface, the interaction nature between adsorbate and substrate is also analyzed by the detailed electronic analysis.

Original language	English
Pages (from-to)	775-781
Number of pages	7
Journal	Langmuir
Volume	26
Issue number	2
DOIs	https://doi.org/10.1021/la9021646
Publication status	Published - 2010 Jan 19

ASJC Scopus subject areas

General Materials Science
Condensed Matter Physics
Surfaces and Interfaces
Spectroscopy
Electrochemistry

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title = "Density functional studies of the adsorption and dissociation of CO 2 molecule on Fe(111) surface",

abstract = "Spin-polarized density functional theory calculation was carried out to characterize the adsorption and dissociation of CO2 molecule on the Fe(111) surface. It was shown that the barriers for the stepwise CO2 dissociation reaction, CO2(g) →C(a) + 2O (a), are 21.73 kcal/mol (for OC-O bond activation) and 23.87 kcal/mol (for C-O bond activation), and the entire process is 35.73 kcal/mol exothermic. The rate constants for the dissociative adsorption of CO2 have been predicted with variational RRKM theory, and the predicted rate constants, k CO2 (in unit of cm3 molecule-1 s-1), can be represented by the equations 2.12 x 10-8T-0.842 exp(-0.258 kcal mol-1/RT) at T = 100-1000 K. To gain insights into high catalytic activity of the Fe(111) surface, the interaction nature between adsorbate and substrate is also analyzed by the detailed electronic analysis.",

author = "Chen, {Hui Lung} and Chen, {Hsin Tsung} and Ho, {Jia Jen}",

year = "2010",

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doi = "10.1021/la9021646",

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journal = "Langmuir",

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T1 - Density functional studies of the adsorption and dissociation of CO 2 molecule on Fe(111) surface

AU - Chen, Hui Lung

AU - Chen, Hsin Tsung

AU - Ho, Jia Jen

PY - 2010/1/19

Y1 - 2010/1/19

N2 - Spin-polarized density functional theory calculation was carried out to characterize the adsorption and dissociation of CO2 molecule on the Fe(111) surface. It was shown that the barriers for the stepwise CO2 dissociation reaction, CO2(g) →C(a) + 2O (a), are 21.73 kcal/mol (for OC-O bond activation) and 23.87 kcal/mol (for C-O bond activation), and the entire process is 35.73 kcal/mol exothermic. The rate constants for the dissociative adsorption of CO2 have been predicted with variational RRKM theory, and the predicted rate constants, k CO2 (in unit of cm3 molecule-1 s-1), can be represented by the equations 2.12 x 10-8T-0.842 exp(-0.258 kcal mol-1/RT) at T = 100-1000 K. To gain insights into high catalytic activity of the Fe(111) surface, the interaction nature between adsorbate and substrate is also analyzed by the detailed electronic analysis.

AB - Spin-polarized density functional theory calculation was carried out to characterize the adsorption and dissociation of CO2 molecule on the Fe(111) surface. It was shown that the barriers for the stepwise CO2 dissociation reaction, CO2(g) →C(a) + 2O (a), are 21.73 kcal/mol (for OC-O bond activation) and 23.87 kcal/mol (for C-O bond activation), and the entire process is 35.73 kcal/mol exothermic. The rate constants for the dissociative adsorption of CO2 have been predicted with variational RRKM theory, and the predicted rate constants, k CO2 (in unit of cm3 molecule-1 s-1), can be represented by the equations 2.12 x 10-8T-0.842 exp(-0.258 kcal mol-1/RT) at T = 100-1000 K. To gain insights into high catalytic activity of the Fe(111) surface, the interaction nature between adsorbate and substrate is also analyzed by the detailed electronic analysis.

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Density functional studies of the adsorption and dissociation of CO ₂ molecule on Fe(111) surface

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