Oscillations in Catalytic Reactions
01 Jan 1977-Catalysis Reviews-science and Engineering (Taylor & Francis Group)-Vol. 15, Iss: 1, pp 107-172
TL;DR: In this article, the status of knowledge concerning open catalytic reaction systems which exhibit sustained oscillatory states was examined, and it was shown that such behavior arouses in the reader that such systems can be easily confused.
Abstract: This paper deals with the status of knowledge concerning open catalytic reaction systems which, though exposed to constant conditions, exhibit sustained oscillatory states. Such behavior arouses in...
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TL;DR: In this paper, the authors present a theoretical explanation for carbon monoxide on platinum catalytic catalytic reactions, which poses difficulties and challenges to both the experimentalist and the theoretician, due to the frequent observations of hysteresis, associated with steady-state multiplicity, and self-sustained oscillations in the reaction.
Abstract: Although the oxidation of carbon monoxide on platinum is one of the oldest known catalytic reactions and one of the most thoroughly studied, it continues to pose difficulties and challenges to both the experimentalist and the theoretician. For the most part, these are due to the frequent observations of hysteresis, associated with steady-state multiplicity, and self-sustained oscillations in the reaction and to the fact that no generally accepted theoretical explanation for them is at hand. even though a large number of studies have addressed the subject.
202 citations
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TL;DR: In this article, the authors focused on the oscillatory catalytic reactions at single-crystal surfaces and explored the elementary steps underlying the complex temporal and spatial effects in fair detail, which information, in turn, could be used for theoretical modeling.
Abstract: Publisher Summary This chapter focuses on the oscillatory catalytic reactions at single-crystal surfaces. Among oscillating chemical systems, catalytic reactions at well-defined single-crystal surfaces under low-pressure conditions are conceptually particularly attractive for the following reasons: The reacting medium is strictly two-dimensional and uniform on the mezoscopic length scale, which is relevant for spatial pattern formation. In addition, the low partial pressures cause only minor heat production by the reaction, so that usually isothermal conditions can be kept to within a very good approximation. By combining kinetic measurements with surface-sensitive techniques, it became possible to explore the elementary steps underlying the complex temporal and spatial effects in fair detail, which information, in turn, then could be used for theoretical modeling. For the systems described in the chapter, the following mechanisms is found to determine the occurrence of isothermal kinetic oscillations: (1) adsorbate driven structural transformation, (2) formation and depletion of a subsurface oxygen species, and (3) autocatalytic surface reaction.
183 citations
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TL;DR: In this paper, a review brings attention to much of the recent literature describing these developments and their applications, particularly regarding complex and chaotic oscillations, as well as reported experimental observations which, in many cases, have provided support for prior theory and in many others, have led to new theoretical developments.
172 citations
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TL;DR: In this paper, the catalytic CO oxidation on Pt(110) under isothermal conditions in a flow reactor was detected and recorded by means of work function measurements between 440 and 590 K and in a pressure range between 10 −5 and 10 −3 Torr.
170 citations
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TL;DR: In this article, the authors reported measurements of the temporal oscillatory oxidation rates of CO over polycrystalline Pt wire and found that the oscillations are believed to occur between two branches of a Langmuir-Hinshelwood reaction mechanism.
141 citations
References
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TL;DR: In this article, the types of dynamic behavior possible for a single first order reaction carried out in a stirred tank reaction are classified according to values of the parameters and plots in parameter space used to define the various possibilites.
655 citations
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TL;DR: In this article, the dynamic behavior of the continuous stirred tank reactor is analyzed and classified for a variable reactor residence time, and plots are given to show the influence of system parameters on the reactor behavior.
241 citations
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TL;DR: In this paper, a supported Pt catalyzed oxidation of CO was studied as a function of sintering severity and sustained isothermal oscillations were observed, which can be rationalized by viewing the oxidation process as one consisting of an Eley-Rideal mechanism involving gaseous CO reacting with adsorbed O 2 at low CO concentrations, and chemisorption of O 2 upon a surface partially covered with CO at higher CO concentrations.
167 citations
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TL;DR: In this article, Zund/Losch-Erscheinungen als einfache Beispiele thermisch verursachter Instabilitaten studiert.
Abstract: Bei der H2-Oxidation an einem einzelnen Katalysatorkorn (Pt auf γ-Al2O3) werden Zund/Losch-Erscheinungen als einfache Beispiele thermisch verursachter Instabilitaten studiert. Unter geeigneten Reaktionsbedingungen tritt oszillatorisches Verhalten auf mit Amplituden der Kornuberhitzung bis zu 60 grd und Schwingungsdauern in der Grosenordnung von Stunden. Bei der katalytischen CO-Oxidation, deren Geschwindigkeit eine fallende Charakteristik aufweist, werden isotherme (kinetisch verursachte) Instabilitaten beobachtet. Dem Zund/Losch-Phanomen entsprechen hier Sprunge zwischen aktiven und inaktiven Zustanden der Katalysatoroberflache. Auch treten isotherme Oszillationen vom Charakter von Kippschwingungen und mit Periodendauern von Minuten auf.
133 citations