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arXiv · 1301.3285

CO oxidation on Pd(100) vs. PdO(sqrt5xsqrt5)R27^o: First-Principles Kinetic Phase Diagrams and Bistability Conditions

Max J. Hoffmann·Karsten Reuter
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Abstract

We present first-principles kinetic Monte Carlo (1p-kMC) simulations addressing the CO oxidation reaction at Pd(100) for gas-phase conditions ranging from ultra-high vacuum (UHV) to ambient pressures and elevated temperatures. For the latter technologically relevant regime there is a long-standing debate regarding the nature of the active surface. The pristine metallic surface, an ultra-thin (sqrt5xsqrt5)R27^o PdO(101) surface oxide, and thicker oxide layers have each been suggested as the active state. We investigate these hypotheses with 1p-kMC simulations focusing on either the Pd(100) surface or the PdO(101) surface oxide and intriguingly obtain a range of (T, p)-conditions where both terminations appear metastable. The predicted bistability regime nicely ties in with oscillatory behavior reported experimentally by Hendriksen and coworkers [Catal. Today 105, 234 (2005)]. Within this regime we find that both surface terminations exhibit very similar intrinsic reactivity, which puts doubts on attempts to assign the catalytic function to just one active state.

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Max J. Hoffmann, Karsten Reuter. 2013-01-15. CO oxidation on Pd(100) vs. PdO(sqrt5xsqrt5)R27^o: First-Principles Kinetic Phase Diagrams and Bistability Conditions. https://doi.org/10.1007/s11244-013-0172-5

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