Oscillating Langmuir−Hinshelwood Mechanisms

Eiswirth, M.; Burger, Jakob; Strasser, Peter; Ertl, G.

doi:10.1021/jp961688y

Cited by 70 publications

(54 citation statements)

References 34 publications

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“…The above condition therefore just represents a precise formulation of the wellknown argument that oscillations can be due to the interplay of a fast autocatalysis and a negative feedback loop occurring on a slower time scale. 13 For the existence proofs we choose a simple combination E 1 + E 2 + E 3 , the corresponding current matrix diagram D CM is also shown in Fig. 1.…”

Section: A Stability Analysismentioning

confidence: 99%

Mechanism and model of the oscillatory electro-oxidation of methanol

Sauerbrei

Nascimento

Eiswirth

et al. 2010

The Journal of Chemical Physics

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Particle-particle particle-mesh method for dipolar interactions: On error estimates and efficiency of schemes with analytical differentiation and mesh interlacing J. Chem. Phys. 135, 184110 (2011) Revisiting falloff curves of thermal unimolecular reactions J. Chem. Phys. 135, 054304 (2011) Collision limited reaction rates for arbitrarily shaped particles across the entire diffusive Knudsen number range J. Chem. Phys. 135, 054302 (2011) Simulating structural transitions by direct transition current sampling: The example of LJ38 J. Chem. Phys. 135, 034108 (2011) Optimizing transition interface sampling simulations J. Chem. Phys. 134, 244118 (2011) Additional information on J. Chem. Phys. A mechanism for the kinetic instabilities observed in the galvanostatic electro-oxidation of methanol is suggested and a model developed. The model is investigated using stoichiometric network analysis as well as concepts from algebraic geometry ͑polynomial rings and ideal theory͒ revealing the occurrence of a Hopf and a saddle-node bifurcation. These analytical solutions are confirmed by numerical integration of the system of differential equations.

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Section: A Stability Analysismentioning

confidence: 99%

Mechanism and model of the oscillatory electro-oxidation of methanol

Sauerbrei

Nascimento

Eiswirth

et al. 2010

The Journal of Chemical Physics

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“…As such, they could form the basis for mathematical descriptions of the oscillatory behavior but not give any precise insight as to the fundamental mechanisms that lay behind them. The progressive work of Ertl and co-workers [47,48,52,[60][61][62][63][64][65][66][67][68] then slowly gained windows into this behavior using probes as PEEM, LEED, and ultimately STM, to reveal a range of possible sources of the oscillatory behavior for well-defined Pt surfaces working at low pressures: whether these same sources were at work in real supported Pt catalysts was still very much a mystery and the subject of much conjecture.…”

Section: Fast X-ray Diffraction (Xrd) and Debye-analysis Of Oscillatimentioning

confidence: 99%

“…As a result, by the 1980s, these phenomena had become the object of intense theoretical and experimental research that resulted in numerous mechanistic possibilities for their explanation , e.g., spatial separation and self-organization of the reactants [48,[60][61][62][63][64][65][66][67][68], surface reconstruction [42,48,[50][51][52]60], surface roughening/retexturing [49], the deposition and then ignition of carbon on the Pt [56][57][58][59], and reversible reduction-oxidation of the Pt itself [39][40][41][43][44][45]49,50].…”

Section: Introductionmentioning

confidence: 99%

“…New spatially resolving methods (notably photoelectron emission microscopy (PEEM) [61,62,64,65] and latterly scanning tunneling microscopy (STM) [68]) started to be developed in the late 1980s and early 1990s and used to progressively detail the structural source of kinetic complexity in CO oxidation on Pt single crystal surfaces with ever greater precision [60][61][62][63][64][65][66][67][68].…”

Section: Introductionmentioning

confidence: 99%

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Time Resolved Operando X-ray Techniques in Catalysis, a Case Study: CO Oxidation by O2 over Pt Surfaces and Alumina Supported Pt Catalysts

Newton

2017

Catalysts

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Abstract:The catalytic oxidation of CO by O 2 to form CO 2 over Pt surfaces and supported catalysts is one of the most studied catalytic reactions from both fundamental and applied points of view. This review aims to show how the application of a range of time resolved, X-ray based techniques, such as X-ray diffraction (XRD), Surface X-ray diffraction (SXRD), total X-ray scattering/pair distribution function (PDF), X-ray absorption (XAFS), X-ray emission (XES), and X-ray photoelectron spectroscopies (XPS), applied under operando conditions and often coupled to adjunct techniques (for instance mass spectrometry (MS) and infrared spectroscopy (IR)) have shed new light on the structures and mechanisms at work in this most studied of systems. The aim of this review is therefore to demonstrate how a fusion of the operando philosophy with the ever augmenting capacities of modern synchrotron sources can lead to new insight and catalytic possibilities, even in the case of a process that has been intensely studied for almost 100 years.

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“…The stoichiometric network analysis developed by Clarke [17] is a powerful tool to study the stability of complex reaction networks. Based on the stoichiometric network analysis, conditions for the occurrence of a Hopf bifurcation in reaction networks are proposed in [18,19].…”

Section: Introductionmentioning

confidence: 99%

A Positive Real Eigenvalue Condition for the Determination of Unstable Steady States in Chemical Reaction Networks

Chao

Chuang

et al. 2008

Zeitschrift Für Naturforschung A

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The interesting dynamical behaviours exhibiting in chemical reaction systems, such as multiple steady states and undamped oscillations, often result from unstable steady states. A positive real eigenvalue condition is proposed which gives a necessary and sufficient condition for the determination of an unstable steady state having a positive real eigenvalue in general isothermal reaction networks. Formulas are developed to construct an unstable steady state and a set of positive rate constants. The applications are illustrated by three examples. Two give rise to oscillations and one admits multiple steady states.

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Oscillating Langmuir−Hinshelwood Mechanisms

Cited by 70 publications

References 34 publications

Mechanism and model of the oscillatory electro-oxidation of methanol

Mechanism and model of the oscillatory electro-oxidation of methanol

Time Resolved Operando X-ray Techniques in Catalysis, a Case Study: CO Oxidation by O2 over Pt Surfaces and Alumina Supported Pt Catalysts

A Positive Real Eigenvalue Condition for the Determination of Unstable Steady States in Chemical Reaction Networks

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