Effect of Temperature in Dynamic Catalysis

Abstract

Nanoparticles have recently been introduced as potentially powerful new catalytic particles. One of the most striking features of nanocatalysts is the dynamic nature of their active sites, which might lead to higher catalytic efficiency compared with traditional static catalysts. However, the microscopic mechanisms underlying the dynamic catalysis processes remain poorly understood. It is also unclear how it can be coupled with other tools to control chemical reactions, such as temperature. Using a recently developed stochastic framework, we investigated the role of temperature in dynamic catalysis. Temperature might have a complex effect on the catalytic properties of a dynamically fluctuating system, depending on the underlying free-energy landscape. Our theoretical approach provides explicit estimates of the properties of catalyzed chemical reactions, allowing us to better understand the microscopic picture of the temperature effect in dynamic catalysis. It is also shown that the dynamic catalysis is a strongly nonequilibrium phenomenon, and the increased efficiency is the result of additional energy dissipation that we can explicitly estimate. Theoretical methods also clarify the stochastic nature of dynamic catalysis by explicitly calculating the fluctuations in dynamic properties. The presented theoretical approach offers novel insights into the microscopic aspects of catalytic processes where dynamic fluctuations of active sites compete with catalyzed chemical reactions.