Kinetics, limit cycles, and mechanism of the ethylene oxidation on platinum

Vayenas, C.G.; Lee, B.; Michaels, James N.

doi:10.1016/0021-9517(80)90005-6

Cited by 119 publications

(66 citation statements)

References 12 publications

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“…In this connection, Vayenas et al (1980Vayenas et al ( , 1981 reported the oxidation of platinum (and its subsequent reduction) to be associated with rate oscillations. Our models do not predict oscillatory behavior without invoking a specific mechanism to do so.…”

Section: Discussionmentioning

confidence: 97%

“…The rate of formation of C 0 2 has been reported by some to exhibit a negative-order dependence on ethylene and a positive-order dependence on oxygen (Cant and Hall, 1970;Hawkins and Wanke, 1979). Others have concluded that the rate dependencies are different for excess ethylene than for conditions involving excess oxygen (Vayenas et al, 1980(Vayenas et al, , 1981. There have been suggestions that different ratedetermining steps are involved in these two situations (CarCorropondcnax concerning this paper should k addrrsscd to E. E. Wol f. berry, 1977).…”

Section: Introductionmentioning

confidence: 93%

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Transient studies and kinetic modeling of ethylene oxidation on Pt/SiO₂

Sant¹,

Kaul²,

Wolf³

1989

AIChE Journal

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This paper describes a reaction-reactor model, utilizing alternative reaction pathways, developed to explain experimental results from the total oxidation of ethylene on a Pt /SO, catalyst. Transient temperature-programmed reaction and concentration-programmed reaction experiments were utilized to study the reaction through FTlR spectroscopic and surface temperature measurements combined with bulk measurements of concentration and temperature. Different elementarystep pathways were incorporated into the concentration and energy balances in performing the simulations. One pathway utilized adsorbed CO, formed from adsorbed ethylene, as the route to CO, formation. This pathway is shown to become important under ethylene-rich conditions. The second pathway utilized the direct reaction between adsorbed ethylene and adsorbed oxygen as the path to CO, formation. The latter route is shown to become important under oxygen-rich conditions. Finally, an example is utilized to show the advantages of the nonequilibrium elementary-step modeling approach over conventional "equilibrium" models where only one step is taken to be rate-determining.

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Section: Discussionmentioning

confidence: 97%

Section: Introductionmentioning

confidence: 93%

Transient studies and kinetic modeling of ethylene oxidation on Pt/SiO₂

Sant¹,

Kaul²,

Wolf³

1989

AIChE Journal

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“…The oscillatory behaviour of the oxidation of ethylene has been extensively investigated on polycrystalline Pt, Rh and Ag catalysts [4,5,[12][13][14][15]. In several cases [4,5,12,13] the technique of solid electrolyte potentiometry (SEP) was used to continuously monitor the activity of oxygen on the catalyst surface during oscillations.…”

Section: Introductionmentioning

confidence: 99%

“…Several heterogeneous catalytic systems operating near the surface oxide stability limit have often been found to exhibit oscillatory behaviour [1][2][3][4][5]. In most cases, oscillations in the reaction rate are observed in the transition region between the two steady-states, characterized by high and low reaction rate [1].…”

Section: Introductionmentioning

confidence: 99%

“…In several cases [4,5,12,13] the technique of solid electrolyte potentiometry (SEP) was used to continuously monitor the activity of oxygen on the catalyst surface during oscillations. In general, the surface oxygen activity and the rate of CO 2 production were found to oscillate simultaneously and in the opposite direction, i.e., a decrease in the activity of surface oxygen always corresponded to an increase in reaction rate.…”

Section: Introductionmentioning

confidence: 99%

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Electrochemically Induced Oscillations of C2H4 Oxidation Over Thin Sputtered Rh Catalyst Films

et al. 2005

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The electrochemically promoted induction of self-sustained catalytic rate and potential oscillations during C 2 H 4 oxidation was studied over sputtered Rh thin (40 nm catalyst films interfaced with ZrO 2 (8 mol% Y 2 O 3 ). The reaction rate oscillates simultaneously with the catalyst potential, and always in the opposite direction. The electrochemically induced oscillatory rate is typically 60 times larger than the open-circuit catalytic rate and 1000 times larger than the electrochemical rate of O 2) supply to the catalyst. The phenomenon is completely reversible and only observed under anodic polarization where the rate oscillates between the values corresponding to metallic Rh and surface Rh 2 O 3 . The oscillations are caused by the electrochemically controlled backspillover of O 2) to the catalyst surface and the concomitant, via repulsive lateral interactions, decomposition of surface rhodium oxide followed by surface reoxidation to Rh 2 O 3 by gaseous O 2 .

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Fabrication and operation of flow‐through tubular SOFCs for electric power and synthesis gas cogeneration from methane

Shi

Yang

et al. 2013

AIChE Journal

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Flow-through type tubular solid oxide fuel cells were successfully fabricated and operated with a single-chamber configuration for realizing the simultaneous generation of electric power and synthesis gas from methane by integrating a downstream catalyst into the fuel cell reactor. A new operation mode, which completely eliminated the gas diffusion between cathode side and anode side, is proposed. The cell showed high open-circuit voltages of 1.02-1.08 V at the furnace temperature range of 650-800 C when operating on CH 4 -O 2 gas mixture at a molar ratio of 2:1. A peak power density of approximately 300 mW cm 22 and a maximum power output of 1.5 W were achieved for a single cell with an effective cathode geometric surface area of 5.4 cm 2 at the furnace temperature of 750 C. The in-situ initialization of the cell using CH 4 -O 2 gas mixture was also realized via applying an effective catalyst into the tubular cell.

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Kinetics, limit cycles, and mechanism of the ethylene oxidation on platinum

Cited by 119 publications

References 12 publications

Transient studies and kinetic modeling of ethylene oxidation on Pt/SiO₂

Transient studies and kinetic modeling of ethylene oxidation on Pt/SiO₂

Electrochemically Induced Oscillations of C2H4 Oxidation Over Thin Sputtered Rh Catalyst Films

Fabrication and operation of flow‐through tubular SOFCs for electric power and synthesis gas cogeneration from methane

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Kinetics, limit cycles, and mechanism of the ethylene oxidation on platinum

Cited by 119 publications

References 12 publications

Transient studies and kinetic modeling of ethylene oxidation on Pt/SiO2

Transient studies and kinetic modeling of ethylene oxidation on Pt/SiO2

Electrochemically Induced Oscillations of C2H4 Oxidation Over Thin Sputtered Rh Catalyst Films

Fabrication and operation of flow‐through tubular SOFCs for electric power and synthesis gas cogeneration from methane

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Product

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Transient studies and kinetic modeling of ethylene oxidation on Pt/SiO₂

Transient studies and kinetic modeling of ethylene oxidation on Pt/SiO₂