Controlling Chemical Turbulence by Global Delayed Feedback: Pattern Formation in Catalytic CO Oxidation on Pt(110)

Kim, Minseok; Bertram, Matthias; Pollmann, Michael; Oertzen, Alexander von; Mikhailov, Alexander S.; Rotermund, Harm Hinrich; Ertl, G.

doi:10.1126/science.1059478

Cited by 378 publications

(214 citation statements)

References 26 publications

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“…It is more probably that the synchronization of separated oscillators over the catalyst surface proceeds via the gas and/or surface diffusion [69,70]. However, in both cases, increasing the reaction rate (or catalyst activity) leads to an increase in the feedback intensity and initiates the appearance of the regular self-sustained oscillations [71].…”

Section: Discussionmentioning

confidence: 99%

Evolution of self-sustained kinetic oscillations in the catalytic oxidation of propane over a nickel foil

Каичев

Teschner

Saraev

et al. 2016

Journal of Catalysis

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The evolution of self-sustained reaction-rate oscillations in the catalytic oxidation of propane over a nickel foil has been studied in situ using X-ray photoelectron spectroscopy coupled with on line mass spectrometry and gas chromatography. Changes in the effective surface area and in the catalyst morphology under reaction conditions have been examined by scanning electron microscopy and a krypton adsorption technique. It is shown that the regular kinetic oscillations arise under oxygen-lean conditions. CO, CO 2 , H 2 , H 2 O, and propylene are detected as products.The conversion of propane oscillates in a range from 1% to 23%. During the half-periods with high activity, the main reaction pathway is the partial oxidation of propane: selectivity toward CO achieves 98%. In contrast, during the half-periods with low activity, the reaction proceeds through three competitive pathways: the partial oxidation of propane, the total oxidation of propane, and the dehydrogenation of propane to propylene. The driving force for the selfsustained kinetic oscillations is the periodic reoxidation of nickel. According to the Ni2p and O1s core-level spectra measured in situ, the high-active catalyst surface is represented by metallic nickel, whereas during the inactive half-periods the catalyst surface is covered with a thick layer of NiO. The intensity of O1s spectra follows the oscillations of O 2 in the gas phase during the oxidation of propane. It is found that during the induction period before the regular oscillations appear, a rough and porous structure develops because of strong reconstruction of the catalyst surface. The thickness of the reconstructed layer is approximately 10-20 µm. This process is accompanied with at least an 80-fold increase in the effective surface area compared with a clean, non-treated nickel foil, which undoubtedly leads to a drastic increase in the number of active sites. We believe that it is the main reason for the induction period always being  Corresponding author.E-mail address: vvk@catalysis.ru (V.V. Kaichev) 2 observed before the appearance of self-sustained oscillations in the catalytic oxidation of light hydrocarbons over catalysts with a low specific surface area (single crystals, foils, or wires).Moreover, without such reconstruction, the oscillations cannot arise due to low activity of such catalysts.

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Section: Discussionmentioning

confidence: 99%

Evolution of self-sustained kinetic oscillations in the catalytic oxidation of propane over a nickel foil

Каичев

Teschner

Saraev

et al. 2016

Journal of Catalysis

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“…Several control strategies have been developed for purposeful manipulation of wave dynamics as the application of closed-loop or feedback-mediated control loops with and without delays [8][9][10][11] and open-loop control that includes external spatio-temporal forcing [10,[12][13][14], optimal control [15][16][17], and control by imposed geometric constraints and heterogeneities on the medium [18,19]. While feedback-mediated control relies on continuously monitoring of the system's state, open-loop control is based on a detailed knowledge of the system's dynamics and its parameters.…”

Section: Introductionmentioning

confidence: 99%

Analytical, Optimal, and Sparse Optimal Control of Traveling Wave Solutions to Reaction-Diffusion Systems

Ryll

Löber

Martens

et al. 2016

Understanding Complex Systems

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Abstract. This work deals with the position control of selected patterns in reactiondiffusion systems. Exemplarily, the Schlögl and FitzHugh-Nagumo model are discussed using three different approaches. First, an analytical solution is proposed. Second, the standard optimal control procedure is applied. The third approach extends standard optimal control to so-called sparse optimal control that results in very localized control signals and allows the analysis of second order optimality conditions.

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“…In particular, the stabilization and control of various patterns [3][4][5][6][7][8][9] through local, nonlocal, or global feedback, and pattern formation in media with designed heterogeneities [10 -12] are the source of novel insights for spatiotemporal dynamics.…”

mentioning

confidence: 99%

Gentle Dragging of Reaction Waves

et al. 2003

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Using a recently realized ''addressable catalyst surface'' [Science 294, 134 (2001)] we study the interaction of chemical reaction waves with prescribed spatiotemporal fields. In particular, we study how a traveling chemical pulse is ''dragged'' by a localized, moving temperature heterogeneity as a function of its intensity and speed. The acceleration and eventual ''detachment'' of the wave from the heterogeneity is also explored through simulation and stability analysis. DOI: 10.1103/PhysRevLett.90.018302 PACS numbers: 82.40.Bj, 05.45.-a, 82.40.Np, 82.45.Jn As the elements of spontaneous pattern formation are progressively understood through theory, experimentation, and scientific computation [1], ways to purposefully interact with the coherent structures (pulses and fronts) that constitute the building blocks of spatiotemporal patterns are becoming the focus of extensive research [2,3]. In particular, the stabilization and control of various patterns [3-9] through local, nonlocal, or global feedback, and pattern formation in media with designed heterogeneities [10 -12] are the source of novel insights for spatiotemporal dynamics.To explore such phenomena, we have recently constructed an ''addressable catalyst'': A focused laser beam, manipulated through computer-controlled mirrors and capable of ''writing'' spatiotemporal temperature heterogeneity patterns on a metal single crystal catalyst. The loop between this actuation and sensing (both resolved in space and time) through nonintrusive microscopies is then closed through the computer or the experimentalist herself/himself in real time. Our model system is the low-pressure catalytic oxidation of CO on Pt(110), a reaction exhibiting well-documented spatiotemporal patterns [13][14][15][16], and whose macroscopic modeling has reached an advanced level [17][18][19][20].In this Letter we study the interaction of reactive pulses with a single, spatially coherent but temporally mobile heterogeneity. In particular, we use a temperature heterogeneity, localized in space and steadily moving in time, to ''drag'' spontaneously isothermally forming reactive pulses and fronts with speeds differing from their natural speed. We examine the shapes acquired by these dragged waves and their limits of stability (that is, the range of dragging speeds for which they can exist). Through computer-aided analysis we examine the nature of the detachment instability, marking the loss of the ability of the heterogeneity to drag a pulse in 1D or 2D. Two possible paths to instability (depending on the linearized spectrum crossing) are detected. We explore the postdetachment transient dynamics and the interactions of a pulse with successive elements of a 1D periodic, constant speed array of identical heterogeneities. The theme of pulse dragging is currently also being explored in a variety of physically relevant Hamiltonian systems, or weakly perturbed dissipative variations thereof (targeted transfer of pulses in optical media or the motion/displacement of harmonic traps or optical l...

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Controlling Chemical Turbulence by Global Delayed Feedback: Pattern Formation in Catalytic CO Oxidation on Pt(110)

Cited by 378 publications

References 26 publications

Evolution of self-sustained kinetic oscillations in the catalytic oxidation of propane over a nickel foil

Evolution of self-sustained kinetic oscillations in the catalytic oxidation of propane over a nickel foil

Analytical, Optimal, and Sparse Optimal Control of Traveling Wave Solutions to Reaction-Diffusion Systems

Gentle Dragging of Reaction Waves

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