Kinetic Modeling for Oscillatory Catalytic Reactions

Sheintuch, Moshe; Schmitz, R.A.

doi:10.1021/bk-1978-0065.ch040

Cited by 15 publications

(3 citation statements)

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“…The authors, and especially Yannis Kevrekidis, wish to acknowledge a debt of gratitude to Prof. Sheintuch for his work over the years in chemical reaction dynamics and nonlinear dynamics more generally. His choice of problems (from the first Sheintuch and Schmitz papers [37] ), his style and approach, and the pervasive quality of his work, have been a reference point and an inspiration over many years and encounters. As Skip Scriven would say, “Excelsior!”.…”

Section: Resultsmentioning

confidence: 99%

Data‐driven Evolution Equation Reconstruction for Parameter‐Dependent Nonlinear Dynamical Systems

Sroczynski

Yair

Talmon

et al. 2018

Israel Journal of Chemistry

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When studying observations of chemical reaction dynamics, closed form equations based on a putative mechanism may not be available. Yet when sufficient data from experimental observations can be obtained, even without knowing what exactly the physical meaning of the parameter settings or recorded variables are, data-driven methods can be used to construct minimal (and in a sense, robust) realizations of the system. The approach attempts, in a sense, to circumvent physical understanding, by building intrinsic “information geometries” of the observed data, and thus enabling prediction without physical/chemical knowledge. Here we use such an approach to obtain evolution equations for a data-driven realization of the original system – in effect, allowing prediction based on the informed interrogation of the agnostically organized observation database. We illustrate the approach on observations of (a) the normal form for the cusp singularity, (b) a cusp singularity for the nonisothermal CSTR, and (c) a random invertible transformation of the nonisothermal CSTR, showing that one can predict even when the observables are not “simply explainable” physical quantities. We discuss current limitations and possible extensions of the procedure.

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Section: Resultsmentioning

confidence: 99%

Data‐driven Evolution Equation Reconstruction for Parameter‐Dependent Nonlinear Dynamical Systems

Sroczynski

Yair

Talmon

et al. 2018

Israel Journal of Chemistry

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“…The formation of subsurface oxygen, coupled with reduction by CO, may lead to kinetic oscillations during the catalytic oxidation of CO on single-crystal Pd(110) , as well as to spatiotemporal pattern formation. Microkinetic models that account for this step have been used successfully to simulate reaction rate oscillations and pattern formation. ,, This mechanism was speculated to occur during CO oxidation on polycrystalline Pt , and Pd and was employed in many studies of pattern-formation …”

Section: Introductionmentioning

confidence: 99%

Subsurface Incorporation of Oxygen into Palladium(111): A Theoretical Study of Energetics and Kinetics

2009

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The kinetic and thermodynamic characteristics of oxygen penetration of palladium (111) surface are studied using the DFT cluster method. The activation energy and the energy difference between the adsorbed and subsurface states of oxygen atom as well as the corresponding frequency and geometrical characteristics are computed from the minimum energy paths describing the penetration process. A simple analytical model of this process is suggested and is applied in order to gain insight into its mechanism and estimate its rate. This approach is used to predict the trends in the activation barriers for the penetration of a single oxygen atom on several transition metals showing Pd to have the lowest barrier (37 kcal/mol as opposed to 44-46 kcal/ mol with Pt, Ru, Rh, and Ir). It is also applied to show that the dependence of the activation energy on the reaction heat is described by the linear BEP relation and that the activation barrier declines with the oxygen coverage of (111) palladium surface.

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“…Several different mechanisms were proposed as the cause of the oscillations such as: dependence of the activation energy of the rate constants on surface coverage [4][5][6], shift between multiple steady states due to slow adsorptiondesorption of an inert species [7,8], periodic oxidationreduction of the surface [9], and surface temperature oscillations [lo]. Unfortunately, in most previous experimental studies the oscillations were followed just by measurements of either gas phase composition or of reaction rate.…”

Section: Introductionmentioning

confidence: 99%

Reaction Rate Oscillations during the Oxidation of Hydrogen on Nickel

Kurtanjek

Sheintuch

Luss

1980

Ber Bunsenges Phys Chem

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Measurements of contact potential difference (CPD) and effluent oxygen concentration were used to monitor oscillations in the surface state and reaction rate during the oxidation of hydrogen over a nickel plate in a continuous flow reactor. CPD measurements indicate that the system oscillates between an active state in which the reduced surface is covered mainly by chemisorbed oxygen and a less active oxidized state. Heat and mass transfer limitations affect the shape, amplitude and period of the oscillations. However, the oscillations do not disappear when transport limitations become negligible.

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Kinetic Modeling for Oscillatory Catalytic Reactions

Cited by 15 publications

References 0 publications

Data‐driven Evolution Equation Reconstruction for Parameter‐Dependent Nonlinear Dynamical Systems

Data‐driven Evolution Equation Reconstruction for Parameter‐Dependent Nonlinear Dynamical Systems

Subsurface Incorporation of Oxygen into Palladium(111): A Theoretical Study of Energetics and Kinetics

Reaction Rate Oscillations during the Oxidation of Hydrogen on Nickel

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