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Dissociative Adsorption of O2 on Clean and CO-Precovered Pt Surfaces

Published online by Cambridge University Press:  01 February 2011

Bin Shan
Affiliation:
stanfordbshan@hotmail.com, Nanostellar Inc, Computational Nanoscience, 1141 Kassel Ter, Sunnyvale, CA, 94089, United States
Ligen Wang
Affiliation:
lgwang@nanostellar.com, Nanostellar Inc, 3696 Haven Ave, Redwood City, CA, 94063, United States
Jangsuk Hyun
Affiliation:
jshyun@nanostellar.com, Nanostellar Inc, 3696 Haven Ave, Redwood City, CA, 94063, United States
Yang Sang
Affiliation:
syang@nanostellar.com, Nanostellar Inc, 3696 Haven Ave, Redwood City, CA, 94063, United States
Yujun Zhao
Affiliation:
yzhao@nanostellar.com, Nanostellar Inc, 3696 Haven Ave, Redwood City, CA, 94063, United States
John B Nicholas
Affiliation:
jnicholas@nanostellar.com, Nanostellar Inc, 3696 Haven Ave, Redwood City, CA, 94063, United States
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Abstract

It is generally accepted that CO oxidation on transition metals follows a Langmuir-Hinshelwood mechanism. The oxidation reaction takes place in two sequential steps where the oxygen molecule first dissociates into atomic oxygen and then reacts with an adsorbed CO to form CO2. One critical question concerning the reaction kinetics under high pressure is the probability of oxygen dissociation on a highly CO covered surface. On bare transition metal surfaces, molecularly adsorbed oxygen readily dissociates with little or no apparent activation barrier. In industrial diesel engine catalysis, the metal surface is initially packed with CO. Subsequent reactions such as oxygen dissociation must take place on a CO covered surface. In this paper, we performed density functional theory (DFT) calculations for O2 dissociation on Pt(111) in the presence of different CO adsorption environments. While several stable O2 molecular precursor states (top-bridge-top, top-fcc-bridge, and top-hcp-bridge) exist on a clean Pt(111) surface, these precursors become endothermic beyond a critical CO coverage of ∼0.44 ML. Furthermore, the reaction path for CO oxidation via dissociated atomic oxygen becomes less favorable at higher CO coverage, primarily due to competitive adsorption and lateral repulsion. It was found that the oxygen dissociation barrier and the binding energies of atomic oxygen are well correlated via the Evans-Polanyi relationship.

Type
Research Article
Copyright
Copyright © Materials Research Society 2008

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References

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