Shining New Light on the Mechanism of Selective Oxidation Catalysis Using Method Development in Transient Spectroscopy

Abstract

Selective oxidation reactions are some of the most important chemical processes, with enormous economic and environmental contributions. Controlling the selectivity remains the greatest challenge, owing to their complexity, with both parallel and consecutive reaction pathways leading to by-products. Their mode of operation over supported and bulk oxide catalysts has been the subject of debate for decades, largely influenced by phenomenological principles. Recently, direct evidence from transient spectroscopy has provided insight into the dynamical nature of selective oxidation catalysts as well as the actively participating surface species and sites of the catalysts, while highlighting important functions of the supporting structure. This perspective presents the implications of these findings for a scientific understanding of the characteristics of selective oxidation reactions as a basis for rational catalyst design. First, the potential of the transient spectroscopic approach is illustrated based on the available literature on selective oxidation reactions. When moving from supported catalysts to bulk oxide systems with their increased level of structural complexity, additional challenges concerning the determination of structure–performance relationships emerge, but these may be tackled successfully in the future in view of current method development