Investigation of CO oxidation transient kinetics on an oxygen pre-covered Au(211) stepped surface

Enrique Samano; Jooho Kim; Bruce E. Koel

doi:10.1007/s10562-008-9815-8

Investigation of CO oxidation transient kinetics on an oxygen pre-covered Au(211) stepped surface

Enrique Samano, Jooho Kim, Bruce E. Koel

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14 Scopus citations

Abstract

The desire to explain the origin(s) of the unexpected catalytic activity of oxide-supported Au nanoparticles for CO oxidation discovered by Haruta and coworkers has stimulated numerous experimental and theoretical studies of Au nanoclusters in the gas phase and on metal oxide supports, and on Au single-crystal surfaces. In order to explore further the reactivity of low-coordination Au step sites, we have performed transient kinetics studies of CO oxidation on an O-precovered, stepped Au(211) single crystal surface. We found behavior similar to that observed previously on flat Au(111) and (110) surfaces; i.e., there is no evidence in these transient kinetics for any special reactivity associatedwith this stepped Au surface. The CO oxidation reaction rate was highly dependent on the initial oxygen coverage, and we determined an apparent activation energy for CO oxidation of -7.0 kJ mol^-1 for θ_O^init = 0.9 ML. Within the Langmuir-Hinschelwood (LH) reaction scheme, we estimate an activation energy of E_LH = 20-43 kJ mol^-1 on this surface for CO oxidation via this pathway. This is somewhat below the value of 67 kJ mol^-1 predicted by recent theoretical calculations.

Original language	English (US)
Pages (from-to)	263-267
Number of pages	5
Journal	Catalysis Letters
Volume	128
Issue number	3-4
DOIs	https://doi.org/10.1007/s10562-008-9815-8
State	Published - Mar 2009
Externally published	Yes

All Science Journal Classification (ASJC) codes

Catalysis
General Chemistry

Keywords

Au(211)
CO oxidation
Chemisorption
Gold
Ozone
Stepped surface
Temperature programmed desorption (TPD)

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10.1007/s10562-008-9815-8

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title = "Investigation of CO oxidation transient kinetics on an oxygen pre-covered Au(211) stepped surface",

abstract = "The desire to explain the origin(s) of the unexpected catalytic activity of oxide-supported Au nanoparticles for CO oxidation discovered by Haruta and coworkers has stimulated numerous experimental and theoretical studies of Au nanoclusters in the gas phase and on metal oxide supports, and on Au single-crystal surfaces. In order to explore further the reactivity of low-coordination Au step sites, we have performed transient kinetics studies of CO oxidation on an O-precovered, stepped Au(211) single crystal surface. We found behavior similar to that observed previously on flat Au(111) and (110) surfaces; i.e., there is no evidence in these transient kinetics for any special reactivity associatedwith this stepped Au surface. The CO oxidation reaction rate was highly dependent on the initial oxygen coverage, and we determined an apparent activation energy for CO oxidation of -7.0 kJ mol-1 for θOinit = 0.9 ML. Within the Langmuir-Hinschelwood (LH) reaction scheme, we estimate an activation energy of ELH = 20-43 kJ mol-1 on this surface for CO oxidation via this pathway. This is somewhat below the value of 67 kJ mol-1 predicted by recent theoretical calculations.",

keywords = "Au(211), CO oxidation, Chemisorption, Gold, Ozone, Stepped surface, Temperature programmed desorption (TPD)",

author = "Enrique Samano and Jooho Kim and Koel, {Bruce E.}",

note = "Funding Information: Acknowledgments This work was supported by the Department of Energy, Office of Basic Energy Sciences, Chemical Sciences Division.",

year = "2009",

month = mar,

doi = "10.1007/s10562-008-9815-8",

language = "English (US)",

volume = "128",

pages = "263--267",

journal = "Catalysis Letters",

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T1 - Investigation of CO oxidation transient kinetics on an oxygen pre-covered Au(211) stepped surface

AU - Samano, Enrique

AU - Kim, Jooho

AU - Koel, Bruce E.

N1 - Funding Information: Acknowledgments This work was supported by the Department of Energy, Office of Basic Energy Sciences, Chemical Sciences Division.

PY - 2009/3

Y1 - 2009/3

N2 - The desire to explain the origin(s) of the unexpected catalytic activity of oxide-supported Au nanoparticles for CO oxidation discovered by Haruta and coworkers has stimulated numerous experimental and theoretical studies of Au nanoclusters in the gas phase and on metal oxide supports, and on Au single-crystal surfaces. In order to explore further the reactivity of low-coordination Au step sites, we have performed transient kinetics studies of CO oxidation on an O-precovered, stepped Au(211) single crystal surface. We found behavior similar to that observed previously on flat Au(111) and (110) surfaces; i.e., there is no evidence in these transient kinetics for any special reactivity associatedwith this stepped Au surface. The CO oxidation reaction rate was highly dependent on the initial oxygen coverage, and we determined an apparent activation energy for CO oxidation of -7.0 kJ mol-1 for θOinit = 0.9 ML. Within the Langmuir-Hinschelwood (LH) reaction scheme, we estimate an activation energy of ELH = 20-43 kJ mol-1 on this surface for CO oxidation via this pathway. This is somewhat below the value of 67 kJ mol-1 predicted by recent theoretical calculations.

AB - The desire to explain the origin(s) of the unexpected catalytic activity of oxide-supported Au nanoparticles for CO oxidation discovered by Haruta and coworkers has stimulated numerous experimental and theoretical studies of Au nanoclusters in the gas phase and on metal oxide supports, and on Au single-crystal surfaces. In order to explore further the reactivity of low-coordination Au step sites, we have performed transient kinetics studies of CO oxidation on an O-precovered, stepped Au(211) single crystal surface. We found behavior similar to that observed previously on flat Au(111) and (110) surfaces; i.e., there is no evidence in these transient kinetics for any special reactivity associatedwith this stepped Au surface. The CO oxidation reaction rate was highly dependent on the initial oxygen coverage, and we determined an apparent activation energy for CO oxidation of -7.0 kJ mol-1 for θOinit = 0.9 ML. Within the Langmuir-Hinschelwood (LH) reaction scheme, we estimate an activation energy of ELH = 20-43 kJ mol-1 on this surface for CO oxidation via this pathway. This is somewhat below the value of 67 kJ mol-1 predicted by recent theoretical calculations.

KW - Au(211)

KW - CO oxidation

KW - Chemisorption

KW - Gold

KW - Ozone

KW - Stepped surface

KW - Temperature programmed desorption (TPD)

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Investigation of CO oxidation transient kinetics on an oxygen pre-covered Au(211) stepped surface

Abstract

All Science Journal Classification (ASJC) codes

Keywords

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