Theoretical Understanding of Dynamic Catalysis

Abstract

Dynamic catalysis is a phenomenon in which the catalytic properties of the system change with time. It has been recently proposed as an alternative to the current widely utilized static catalytic approach because of potential significant improvements in catalytic efficiency. Dynamic restructuring of active sites on surfaces has also been observed in some nanocatalysts. However, the microscopic mechanisms of underlying processes remain not well understood. We developed a new stochastic framework that allows us to quantitatively describe dynamic catalysis and compare its properties with the static approach. It is found that fluctuations between different catalytic pathways might lead to enhancements in chemical reaction rates but only for specific ranges of kinetic parameters. Our theoretical method can explain these observations from the microscopic point of view. We show that the temporal efficiency of dynamic catalysis depends only on the rates of chemical reactions and transitions between different catalytic pathways while being independent of the number of active sites. It is also argued that the effects of dynamic catalysis are purely nonequilibrium, and the associated energy dissipation is the source of improvements in catalytic efficiency. In addition, the stochasticity of dynamic catalysis is investigated. The proposed theoretical approach clarifies some important microscopic aspects of catalytic processes.