Escaping the trap of complication and complexity in multiscale microkinetic modelling of heterogeneous catalytic...

In this feature article, the development of methods to enable a hierarchical multiscale approach to the microkinetic analysis of heterogeneous catalytic processes is reviewed. This methodology is an effective route to escape the trap of complication and complexity in multiscale microkinetic modelling. On the one hand, the complication of the problem is related to the fact that the observed catalyst functionality is inherently a multiscale property of the reacting system and its analysis requires bridging the phenomena at different time and length scales. On the other hand, the complexity of the problem derives from the system dimension of the chemical systems, which typically results in a number of elementary steps and species, that are beyond the limit of accessibility of present-day computational power even for the most efficient implementation of atomistic first-principles simulations. The main idea behind the hierarchical approach is to tackle the problem with methods of increasing accuracy in a dual feed-back loop between theory and experiments. The potential of the methodology is shown in the context of unravelling the WGS and r-WGS catalytic mechanisms on Rh catalysts. As a perspective, the extension to structure-dependent microkinetic modelling is discussed.