Global and non-local coupling in oscillating heterogeneous catalytic reactions: The oxidation of CO on zeolite supported palladium

Slinko, M. M.; Ukharskii, A. A.; Jaeger, N. I.

doi:10.1039/b005400n

Cited by 17 publications

(13 citation statements)

References 10 publications

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“…33 At pressures higher than 10 –4 mbar, gas-phase coupling provides the synchronization over macroscopic samples, 49,50 and near atmospheric pressure, heat transfer contributes significantly or even dominates spatial coupling. 51,52 Evidently, under the present pressure conditions, the micrometer size of the individual grains is not sufficient to synchronize the kinetic transitions on differently oriented grains via fast CO and oxygen consumption from the gas phase. On the other hand, the grain boundaries seem to hinder effectively the diffusion coupling (frames 1–3 in Figure 5).…”

Section: Resultsmentioning

confidence: 91%

The Role of Defects in the Local Reaction Kinetics of CO Oxidation on Low-Index Pd Surfaces

Vogel

Spiel²,

Schmid³

et al. 2013

J. Phys. Chem. C

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The role of artificially created defects and steps in the local reaction kinetics of CO oxidation on the individual domains of a polycrystalline Pd foil was studied by photoemission electron microscopy (PEEM), mass spectroscopy (MS), and scanning tunneling microscopy (STM). The defects and steps were created by STM-controlled Ar+ sputtering and the novel PEEM-based approach allowed the simultaneous determination of local kinetic phase transitions on differently oriented μm-sized grains of a polycrystalline sample. The independent (single-crystal-like) reaction behavior of the individual Pd(hkl) domains in the 10–5 mbar pressure range changes upon Ar+ sputtering to a correlated reaction behavior, and the reaction fronts propagate unhindered across the grain boundaries. The defect-rich surface shows also a significantly higher CO tolerance as reflected by the shift of both the global (MS-measured) and the local (PEEM-measured) kinetic diagrams toward higher CO pressure.

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Section: Resultsmentioning

confidence: 91%

The Role of Defects in the Local Reaction Kinetics of CO Oxidation on Low-Index Pd Surfaces

Vogel

Spiel²,

Schmid³

et al. 2013

J. Phys. Chem. C

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“…For instance, heterogeneous catalysts for CO oxidation often consist of pellets that have a size distribution. 42 The gas-phase or the heat transfer coupling (with support of high thermal conductivity) is affected by pellet sizes and thus, in addition to kinetic and thermodynamic effects of particle sizes, coupling effects could also alter the global dynamical response of the reacting system. 41,42 The dual oscillator setup with different electrode sizes can be extended to build small sets (e.g.…”

Section: Discussionmentioning

confidence: 99%

“…42 The gas-phase or the heat transfer coupling (with support of high thermal conductivity) is affected by pellet sizes and thus, in addition to kinetic and thermodynamic effects of particle sizes, coupling effects could also alter the global dynamical response of the reacting system. 41,42 The dual oscillator setup with different electrode sizes can be extended to build small sets (e.g. three locally coupled 69,70 ) or large population 21,25 of electrochemical oscillators with asymmetrical coupling.…”

Section: Discussionmentioning

confidence: 99%

“…9,10 When concentrations (or reaction rates) in these units exhibit oscillatory behavior, the interactions can produce a wide array of synchronization related behaviors, e.g., periodic 4,11,12 and chaotic 13,14 synchronization, oscillator death, [15][16][17][18][19][20] collective synchronization, [21][22][23] dynamical clustering, [24][25][26] and quorum transition. 27 The synchronization behaviors have been observed in BelousovZhabotinsky (BZ) reaction, 3,4,12,13,15,28,29 pH oscillators, 30 and biochemical reaction 31 in coupled continuously fed, stirred tank reactors (CSTRs), in metal dissolution 21,24,25,[32][33][34][35][36][37] and electrocatalytic [38][39][40] reactions in electrochemical systems, in CO oxidation on heterogeneous catalysts, 41,42 and in BZ beads, 22,23,26,…”

Section: Introductionmentioning

confidence: 99%

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Dynamics of electrochemical oscillators with electrode size disparity: asymmetrical coupling and anomalous phase synchronization

Wickramasinghe

Mrugacz

Kiss

2011

Phys. Chem. Chem. Phys.

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Experiments are carried out in dual electrode oscillatory Ni electrodissolution in which the two electrodes have different surface areas. The transition to phase synchronization is analyzed as asymmetrical coupling strength, induced by placing a cross resistance between the electrodes, is varied. It is shown that because of nonisochronicity (phase shear, i.e., strong dependence of period on amplitude) of the oscillators, anomalous phase synchronization effects can be observed: advanced/delayed synchronization and, to a lesser extent, frequency difference enhancement. The type of synchronization is strongly affected by the underlying heterogeneities of the oscillators; in the experiments with a slow driver (large surface area) electrode the synchronization is advanced, with a fast driver electrode the synchronization is delayed with respect to symmetrical coupling. The findings thus reveal that the interplay of asymmetrical coupling with the types of inherent heterogeneities plays an important role for the interpretation of size effects in the dynamical behavior of a nonlinear chemical reaction.

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“…Figure 2 shows oscillations under T ¼ 500 K and P CO ¼ 2.5 mm Hg. These values are reported experimentally to show oscillations (Slinko et al, 2001b).…”

Section: Resultsmentioning

confidence: 83%

Bursting on Co Oxidation in a Tubular Reactor

Soto

Caballero

Vicente

2009

Chemical Engineering Communications

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In this work we study CO oxidation by numerical simulation; we used the monocrystal STM model (Sales et al., 1982;Slinko et al., 1999) and extended it to scale on a monolithic tubular reactor. The final model is a mixed system with ordinary and partial differential equations. We found that there is periodic behavior at earlier times, but the simulations at long time show bursting, which appeared as a route to chaotic behavior. Our results can be compared indirectly with a continuous flow reactor under isothermal conditions (Ballandis and Plath, 2000).

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Global and non-local coupling in oscillating heterogeneous catalytic reactions: The oxidation of CO on zeolite supported palladium

Cited by 17 publications

References 10 publications

The Role of Defects in the Local Reaction Kinetics of CO Oxidation on Low-Index Pd Surfaces

The Role of Defects in the Local Reaction Kinetics of CO Oxidation on Low-Index Pd Surfaces

Dynamics of electrochemical oscillators with electrode size disparity: asymmetrical coupling and anomalous phase synchronization

Bursting on Co Oxidation in a Tubular Reactor

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