Surface restructuring and aperiodic kinetic oscillations in heterogeneous catalytic reactions

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摘要：

We present comprehensive Monte Carlo simulations of aperiodic kinetic oscillations in catalytic reactions accompanied by adsorbate-induced surface restructuring. Our analysis, focused on the NO–H 2 reaction on Pt(1 0 0), is based on a lattice-gas model describing surface restructuring in terms of the statistical theory of first-order phase transitions. The oscillations predicted are proved to be robust. In particular, the type of irregularities observed in the reaction kinetics is nearly independent of the used boundary conditions and does not change upon increasing the rate of adsorbate diffusion. On the other hand, the kinetics are found to be very sensitive to small perturbations in the arrangement of adsorbed particles. Specifically, the divergence of the kinetic curves corresponding to slightly different initial conditions occurs very rapidly. The latter indicates that the oscillations obtained can be classified as chaotic.

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Theoretical or Mathematical/ adsorbed layers adsorption catalysis chaos chemical equilibrium hydrogen neutral molecules lattice gas Monte Carlo methods nitrogen compounds platinum reaction kinetics theory surface chemistry surface reconstruction/ aperiodic kinetic oscillations heterogeneous catalytic reactions Monte Carlo simulations adsorbate-induced surface restructuring Pt(100) surface NO-H 2 reaction lattice-gas model statistical theory first-order phase transitions reaction kinetics adsorbate diffusion rate kinetic curves divergence initial conditions chaotic oscillations Pt NO H 2 NO-H 2/ A8265J Heterogeneous catalysis at surfaces and other surface reactions A0545 Theory and models of chaotic systems A0550 Lattice theory and statistics Ising problems A6820 Solid surface structure A6842 Surface phase transitions and critical phenomena A8260H Chemical equilibria and equilibrium constants A8265M Sorption and accommodation coefficients (surface chemistry) A8220D Statistic