Model for the catalytic oxidation of CO, including gas-phase impurities and CO desorption

TL;DR

This study uses kinetic Monte Carlo simulations to explore how gas-phase impurities and CO desorption influence catalytic oxidation of CO, revealing that CO desorption can mitigate impurity effects and sustain catalytic activity.

Contribution

It introduces a modified Ziff-Gulari-Barshad model including impurities and CO desorption, demonstrating their combined impact on catalytic reaction phases and reactivity.

Findings

CO desorption widens the reactive window

Impurities reduce CO_2 production without desorption

Desorption counteracts impurity effects, maintaining activity

Abstract

We present results of kinetic Monte Carlo simulations of a modified Ziff-Gulari-Barshad model for the reaction CO+O --> CO_2 on a catalytic surface. Our model includes impurities in the gas phase, CO desorption, and a modification known to eliminate the unphysical O poisoned phase. The impurities can adsorb and desorb on the surface, but otherwise remain inert. In a previous work that did not include CO desorption [G. M. Buendia and P. A. Rikvold, Phys. Rev. E, 85 031143 (2012)], we found that the impurities have very distinctive effects on the phase diagram and greatly diminish the reactivity of the system. If the impurities do not desorb, once the system reaches a stationary state, the CO_2 production disappears. When the impurities are allowed to desorb, there are regions where the CO_2 reaction window reappears, although greatly reduced. Following experimental evidence that indicates that temperature effects are crucial in many catalytic processes, here we further analyze these effects by including a CO desorption rate. We find that the CO desorption has the effect to smooth the transition between the reactive and the CO rich phase, and most importantly it can counteract the negative effects of the presence of impurities by widening the reactive window such that now the system remains catalytically active in the whole range of CO pressures.