期刊
TOPICS IN CATALYSIS
卷 57, 期 1-4, 页码 159-170出版社
SPRINGER/PLENUM PUBLISHERS
DOI: 10.1007/s11244-013-0172-5
关键词
First-principles kinetic Monte Carlo; Bistability; CO oxidation catalysis; Density-functional theory; In situ characterization
资金
- German Research Council (DFG)
- TUM Faculty Graduate Center Chemistry
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 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 (root 5 x root 5)R27 degrees 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 et al. (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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