Dft study of trichloroethylene chemisorption to iron surfaces using density functional theory

Paul Blowers, Nianliu Zhang, James Farrell

Research output: Chapter in Book/Report/Conference proceedingConference contribution

Abstract

The mechanisms for chemical adsorption of trichloroethylene (TCE) to iron surfaces were studied using periodic density functional theory (DFT). DFT modeling of adsorbed species was performed using the generalized gradient approximation with the Perdew-Burke-Enzerhof (PBE) functional. Chemisorption structures were obtained for four adsorbed initial configurations. Di-sigma C-Fe and Cl-Fe complexes were formed by initial configurations with two carbon (C-bridge) or two chlorine atoms (Cl-bridge) adsorbed at bridge sites between adjacent iron atoms, respectively. Calculated binding energies indicated that chemisorption was highly exothermic, with the complex formed at the C-bridge site being the most energetically favorable. Chemisorption at the C-bridge site had an early transition state in which all three C-Cl bonds were activated from ∼ 1.7 to ∼ 2.2 Å, with an activation energy of 50 kJ/mole. The early transition state and the loss of all three Cl atoms upon chemisorption were consistent with most experimental observations that TCE undergoes complete dechlorination in one interaction with the iron surface. This is an abstract of a paper presented at the AIChE Annual Meeting and Fall Showcase (Cincinnati, OH 1/04/2005).

Original languageEnglish (US)
Title of host publicationAIChE Annual Meeting Conference Proceedings
PublisherAmerican Institute of Chemical Engineers
Volume2005
ISBN (Print)0816909962, 9780816909964
StatePublished - 2005
Externally publishedYes
Event05AIChE: 2005 AIChE Annual Meeting and Fall Showcase - Cincinnati, OH, United States
Duration: Oct 30 2005Nov 4 2005

Other

Other05AIChE: 2005 AIChE Annual Meeting and Fall Showcase
CountryUnited States
CityCincinnati, OH
Period10/30/0511/4/05

Fingerprint

Trichloroethylene
Chemisorption
Density functional theory
Iron
Atoms
Dechlorination
Binding energy
Chlorine
Activation energy
Adsorption
Carbon

ASJC Scopus subject areas

  • Energy(all)

Cite this

Blowers, P., Zhang, N., & Farrell, J. (2005). Dft study of trichloroethylene chemisorption to iron surfaces using density functional theory. In AIChE Annual Meeting Conference Proceedings (Vol. 2005). American Institute of Chemical Engineers.

Dft study of trichloroethylene chemisorption to iron surfaces using density functional theory. / Blowers, Paul; Zhang, Nianliu; Farrell, James.

AIChE Annual Meeting Conference Proceedings. Vol. 2005 American Institute of Chemical Engineers, 2005.

Research output: Chapter in Book/Report/Conference proceedingConference contribution

Blowers, P, Zhang, N & Farrell, J 2005, Dft study of trichloroethylene chemisorption to iron surfaces using density functional theory. in AIChE Annual Meeting Conference Proceedings. vol. 2005, American Institute of Chemical Engineers, 05AIChE: 2005 AIChE Annual Meeting and Fall Showcase, Cincinnati, OH, United States, 10/30/05.
Blowers P, Zhang N, Farrell J. Dft study of trichloroethylene chemisorption to iron surfaces using density functional theory. In AIChE Annual Meeting Conference Proceedings. Vol. 2005. American Institute of Chemical Engineers. 2005
Blowers, Paul ; Zhang, Nianliu ; Farrell, James. / Dft study of trichloroethylene chemisorption to iron surfaces using density functional theory. AIChE Annual Meeting Conference Proceedings. Vol. 2005 American Institute of Chemical Engineers, 2005.
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abstract = "The mechanisms for chemical adsorption of trichloroethylene (TCE) to iron surfaces were studied using periodic density functional theory (DFT). DFT modeling of adsorbed species was performed using the generalized gradient approximation with the Perdew-Burke-Enzerhof (PBE) functional. Chemisorption structures were obtained for four adsorbed initial configurations. Di-sigma C-Fe and Cl-Fe complexes were formed by initial configurations with two carbon (C-bridge) or two chlorine atoms (Cl-bridge) adsorbed at bridge sites between adjacent iron atoms, respectively. Calculated binding energies indicated that chemisorption was highly exothermic, with the complex formed at the C-bridge site being the most energetically favorable. Chemisorption at the C-bridge site had an early transition state in which all three C-Cl bonds were activated from ∼ 1.7 to ∼ 2.2 {\AA}, with an activation energy of 50 kJ/mole. The early transition state and the loss of all three Cl atoms upon chemisorption were consistent with most experimental observations that TCE undergoes complete dechlorination in one interaction with the iron surface. This is an abstract of a paper presented at the AIChE Annual Meeting and Fall Showcase (Cincinnati, OH 1/04/2005).",
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N2 - The mechanisms for chemical adsorption of trichloroethylene (TCE) to iron surfaces were studied using periodic density functional theory (DFT). DFT modeling of adsorbed species was performed using the generalized gradient approximation with the Perdew-Burke-Enzerhof (PBE) functional. Chemisorption structures were obtained for four adsorbed initial configurations. Di-sigma C-Fe and Cl-Fe complexes were formed by initial configurations with two carbon (C-bridge) or two chlorine atoms (Cl-bridge) adsorbed at bridge sites between adjacent iron atoms, respectively. Calculated binding energies indicated that chemisorption was highly exothermic, with the complex formed at the C-bridge site being the most energetically favorable. Chemisorption at the C-bridge site had an early transition state in which all three C-Cl bonds were activated from ∼ 1.7 to ∼ 2.2 Å, with an activation energy of 50 kJ/mole. The early transition state and the loss of all three Cl atoms upon chemisorption were consistent with most experimental observations that TCE undergoes complete dechlorination in one interaction with the iron surface. This is an abstract of a paper presented at the AIChE Annual Meeting and Fall Showcase (Cincinnati, OH 1/04/2005).

AB - The mechanisms for chemical adsorption of trichloroethylene (TCE) to iron surfaces were studied using periodic density functional theory (DFT). DFT modeling of adsorbed species was performed using the generalized gradient approximation with the Perdew-Burke-Enzerhof (PBE) functional. Chemisorption structures were obtained for four adsorbed initial configurations. Di-sigma C-Fe and Cl-Fe complexes were formed by initial configurations with two carbon (C-bridge) or two chlorine atoms (Cl-bridge) adsorbed at bridge sites between adjacent iron atoms, respectively. Calculated binding energies indicated that chemisorption was highly exothermic, with the complex formed at the C-bridge site being the most energetically favorable. Chemisorption at the C-bridge site had an early transition state in which all three C-Cl bonds were activated from ∼ 1.7 to ∼ 2.2 Å, with an activation energy of 50 kJ/mole. The early transition state and the loss of all three Cl atoms upon chemisorption were consistent with most experimental observations that TCE undergoes complete dechlorination in one interaction with the iron surface. This is an abstract of a paper presented at the AIChE Annual Meeting and Fall Showcase (Cincinnati, OH 1/04/2005).

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