Fluctuations and critical phenomena in catalytic CO oxidation on nanoscale Pt facets
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Ames National Laboratory is a government-owned, contractor-operated national laboratory of the U.S. Department of Energy (DOE), operated by and located on the campus of Iowa State University in Ames, Iowa.
For more than 70 years, the Ames National Laboratory has successfully partnered with Iowa State University, and is unique among the 17 DOE laboratories in that it is physically located on the campus of a major research university. Many of the scientists and administrators at the Laboratory also hold faculty positions at the University and the Laboratory has access to both undergraduate and graduate student talent.
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Abstract
Local fluctuations and fluctuation-induced transitions in catalytic CO oxidation are studied with field electron microscopy on the (112) facets of a [100]-oriented Pt field emitter tip. The reaction is investigated in the bistable range close to the cusp point (critical point) that terminates the bistability range in pCO, T-parameter space. The amplitude and the spatial coherence of the fluctuations increase on approaching the critical point. The fluctuations are spatially well correlated on each flat (112) facet, but their correlation decays rapidly across stepped regions that terminate the flat facets. On smaller (112) facets, an onset of fluctuation-induced transitions is observed earlier (i.e., further away from the critical point) than for larger (112) facets. The behavior of the reaction system near the cusp point appears to be similar to that of an equilibrium system near the critical point. The observed fluctuations are mimicked in a simple reaction model for CO oxidation on surfaces that incorporates both rapid diffusion of adsorbed CO, and superlattice ordering of adsorbed immobile oxygen. The steady states of the model exhibit a cusp bifurcation, from a regime of bistability to one of monostability. The fluctuations increase near this cusp point, as in experiment. This behavior is analyzed via kinetic Monte Carlo simulations and analytic procedures, focusing on the consequences for fluctuation-induced transitions.
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This article is from Physical Review B 63 (2001): 165417, doi:10.1103/PhysRevB.63.165417 .