Elucidating the role of extended surface defects at Fe surfaces on CO adsorption and dissociation

Aurab Chakrabarty, El Tayeb Bentria, Salawu Akande Omotayo, Othmane Bouhali, Normand Mousseau, Charlotte S. Becquart, Fadwa El-Mellouhi

Research output: Contribution to journalArticle

Abstract

The adsorption and dissociation of hydrocarbons on metallic surfaces during catalytic reactions in a steam reforming furnace often lead to the carburization of the catalysts and metallic surfaces involved. This process is greatly accelerated by the presence of intrinsic defects like vacancies and grain boundaries and is succeeded by surface to subsurface diffusion of C. We employ both density functional theory and reactive force field molecular dynamics simulations to investigate the effect of surface defects on CO dissociation rate directly related to metal dusting corrosion. We demonstrate that stable surface vacancy clusters with large binding energies accelerate the adsorption of CO molecules by decreasing the corresponding dissociation energies. In addition, we demonstrate that the appearance of multiple GBs at the surface leads to an enhancement of the CO dissociation rate. Furthermore, we demonstrate that the increase in surface roughness by emerging GBs leads to an increase in CO dissociation rate.

Original languageEnglish
Pages (from-to)792-798
Number of pages7
JournalApplied Surface Science
Volume491
DOIs
Publication statusPublished - 15 Oct 2019

Fingerprint

Surface defects
surface defects
Carbon Monoxide
dissociation
Adsorption
adsorption
Vacancies
Steam reforming
Hydrocarbons
Binding energy
steam
field theory (physics)
Density functional theory
furnaces
Molecular dynamics
emerging
corrosion
surface roughness
Grain boundaries
Furnaces

Keywords

  • CO adsorption
  • CO dissociation
  • Grain boundary
  • Iron surface
  • Metal dusting corrosion
  • Reactive force field
  • Surface vacancy clusters

ASJC Scopus subject areas

  • Chemistry(all)
  • Condensed Matter Physics
  • Physics and Astronomy(all)
  • Surfaces and Interfaces
  • Surfaces, Coatings and Films

Cite this

Elucidating the role of extended surface defects at Fe surfaces on CO adsorption and dissociation. / Chakrabarty, Aurab; Bentria, El Tayeb; Omotayo, Salawu Akande; Bouhali, Othmane; Mousseau, Normand; Becquart, Charlotte S.; El-Mellouhi, Fadwa.

In: Applied Surface Science, Vol. 491, 15.10.2019, p. 792-798.

Research output: Contribution to journalArticle

Chakrabarty, Aurab ; Bentria, El Tayeb ; Omotayo, Salawu Akande ; Bouhali, Othmane ; Mousseau, Normand ; Becquart, Charlotte S. ; El-Mellouhi, Fadwa. / Elucidating the role of extended surface defects at Fe surfaces on CO adsorption and dissociation. In: Applied Surface Science. 2019 ; Vol. 491. pp. 792-798.
@article{bed0f674453941c69699371539ac4985,
title = "Elucidating the role of extended surface defects at Fe surfaces on CO adsorption and dissociation",
abstract = "The adsorption and dissociation of hydrocarbons on metallic surfaces during catalytic reactions in a steam reforming furnace often lead to the carburization of the catalysts and metallic surfaces involved. This process is greatly accelerated by the presence of intrinsic defects like vacancies and grain boundaries and is succeeded by surface to subsurface diffusion of C. We employ both density functional theory and reactive force field molecular dynamics simulations to investigate the effect of surface defects on CO dissociation rate directly related to metal dusting corrosion. We demonstrate that stable surface vacancy clusters with large binding energies accelerate the adsorption of CO molecules by decreasing the corresponding dissociation energies. In addition, we demonstrate that the appearance of multiple GBs at the surface leads to an enhancement of the CO dissociation rate. Furthermore, we demonstrate that the increase in surface roughness by emerging GBs leads to an increase in CO dissociation rate.",
keywords = "CO adsorption, CO dissociation, Grain boundary, Iron surface, Metal dusting corrosion, Reactive force field, Surface vacancy clusters",
author = "Aurab Chakrabarty and Bentria, {El Tayeb} and Omotayo, {Salawu Akande} and Othmane Bouhali and Normand Mousseau and Becquart, {Charlotte S.} and Fadwa El-Mellouhi",
year = "2019",
month = "10",
day = "15",
doi = "10.1016/j.apsusc.2019.05.278",
language = "English",
volume = "491",
pages = "792--798",
journal = "Applied Surface Science",
issn = "0169-4332",
publisher = "Elsevier",

}

TY - JOUR

T1 - Elucidating the role of extended surface defects at Fe surfaces on CO adsorption and dissociation

AU - Chakrabarty, Aurab

AU - Bentria, El Tayeb

AU - Omotayo, Salawu Akande

AU - Bouhali, Othmane

AU - Mousseau, Normand

AU - Becquart, Charlotte S.

AU - El-Mellouhi, Fadwa

PY - 2019/10/15

Y1 - 2019/10/15

N2 - The adsorption and dissociation of hydrocarbons on metallic surfaces during catalytic reactions in a steam reforming furnace often lead to the carburization of the catalysts and metallic surfaces involved. This process is greatly accelerated by the presence of intrinsic defects like vacancies and grain boundaries and is succeeded by surface to subsurface diffusion of C. We employ both density functional theory and reactive force field molecular dynamics simulations to investigate the effect of surface defects on CO dissociation rate directly related to metal dusting corrosion. We demonstrate that stable surface vacancy clusters with large binding energies accelerate the adsorption of CO molecules by decreasing the corresponding dissociation energies. In addition, we demonstrate that the appearance of multiple GBs at the surface leads to an enhancement of the CO dissociation rate. Furthermore, we demonstrate that the increase in surface roughness by emerging GBs leads to an increase in CO dissociation rate.

AB - The adsorption and dissociation of hydrocarbons on metallic surfaces during catalytic reactions in a steam reforming furnace often lead to the carburization of the catalysts and metallic surfaces involved. This process is greatly accelerated by the presence of intrinsic defects like vacancies and grain boundaries and is succeeded by surface to subsurface diffusion of C. We employ both density functional theory and reactive force field molecular dynamics simulations to investigate the effect of surface defects on CO dissociation rate directly related to metal dusting corrosion. We demonstrate that stable surface vacancy clusters with large binding energies accelerate the adsorption of CO molecules by decreasing the corresponding dissociation energies. In addition, we demonstrate that the appearance of multiple GBs at the surface leads to an enhancement of the CO dissociation rate. Furthermore, we demonstrate that the increase in surface roughness by emerging GBs leads to an increase in CO dissociation rate.

KW - CO adsorption

KW - CO dissociation

KW - Grain boundary

KW - Iron surface

KW - Metal dusting corrosion

KW - Reactive force field

KW - Surface vacancy clusters

UR - http://www.scopus.com/inward/record.url?scp=85068105283&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=85068105283&partnerID=8YFLogxK

U2 - 10.1016/j.apsusc.2019.05.278

DO - 10.1016/j.apsusc.2019.05.278

M3 - Article

AN - SCOPUS:85068105283

VL - 491

SP - 792

EP - 798

JO - Applied Surface Science

JF - Applied Surface Science

SN - 0169-4332

ER -