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"CO oxidation on thin Pt crystals : stoichiometric and mathematical models."

Bogdan Gnativ 1Myhaylo V. Tokarchuk 2Igor Penyak 1

1. National University "Lvivska Polytechnika", Bendera St. 12, Lviv UA-79013, Ukraine
2. Institute for Condensed Matter Physics of the National Academy of Sciences of Ukraine (ICMP), 1, Sventsitskii, Lviv 79011, Ukraine

Abstract

The problem of developing a mathematical model of oscillatory chemical reactions accompanied by formation of chemically unstable compounds retains importance in kinetics of heterogenic systems. Oxidation of CO on Pt (110) surface is a typical example of such reaction. We performed a stoichiometric analysis of the system in order to simplify the analysis of the process and view it as a sequence of separate elementary stages for which it is easy to determine its numeric characteristics.We applied the concept of formation of active intermediate substances (coating) as reagents in elementary stages of the reaction, avoided the analysis of mass transfer processes, took into account the route of reaction, and built and analysed the stoichiometric matrix. Further, we elaborated a molecular matrix for reaction components. With regard to additional limitations of the mass balance due to the molecular matrix we determined the quantity of linearly independent stages of the process. Linking of rates of elementary reactions with rates of reaction for each component according to the principle of independent elementary reactions lead us to the system of algebraic kinetic equations. In closed systems including each elementary stage of a complex oxidation reaction, it transforms into a system of differential equations. After equalization of elementary stages of the process based on the concept of stoichiometric multipliers in order to avoid the side products of reaction in the final equation and after introduction of corresponding changes into the stoichiometric matrix according to the principles of formal kinetics we obtained the final model for quantitative investigation of time characteristics of complex heterogenic processes in kinetic part. Comparison of quantitative results of model investigation with experimental data indicates that this model can be justifiably applied for processes in kinetic part of experiments.

 

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Related papers

Presentation: poster at E-MRS Fall Meeting 2004, Symposium I, by Igor Penyak
See On-line Journal of E-MRS Fall Meeting 2004

Submitted: 2004-04-30 10:55
Revised:   2009-06-08 12:55