Transformations of Organic Molecules over Metal Surfaces: Insights from Computational Catalysis

Much-needed progress in catalytic science, in particular regarding heterogeneous catalysis, is associated with the transition from largely empirical research to rational design of new and improved catalysts and catalytic processes. To achieve this goal, fundamental atomic-scale understanding of catalytic processes is required, which can be achieved with the help of theoretical modeling, in particular, using methods based on quantum chemical calculations. In this review we illustrate the current progress by discussing examples from the authors’ work in which complex reaction networks involving organic molecules on transition-metal surfaces have been studied using density functional theory. We review some of the success stories where theory helped to interpret experimental observations and provided atomistic insights into the mechanisms, which were not definitively known before. In other cases, partial disagreement between theoretical results and existing experimental evidence calls for further reconciliation studies.