Seeing clear where others are can’t – X-rays uncover the birth of C-H activation catalysts and how they function

Research question

The aim of this proposal is to demonstrate that time-resolved X-ray spectroscopy is a unique method to reveal what determines reactivity of metal-based homogeneous C-H activation catalysts. By probing the metal in transition-metal hydride catalysts in solution, we will follow in real time of the reactions how the catalyst becomes reactive and how it functions to ultimately cleave C-H bonds in hydrocarbon molecules from solution. Extrapolating from our current work with X-ray spectroscopy, addressing the metalspecific orbital interactions with X-ray spectroscopy appears to be the only way to reveal themechanism of C-H activation with metal hydride catalysts, information that cannot, in particular, be attained with time-resolved infrared spectroscopy.

Sustainability aspects

The project proposed here will uncover hitherto inaccessible information on the mechanism of C-H activation catalysts at the ultimate quantum-mechanical level of orbital interactions. This will inform strategies for both chemical synthesis and theoretical predictions for the modification of existing and the design of new catalysts for the activation and functionalization of C-H bonds. The results of the proposed investigations will help developing new ways for the targeted synthesis of high-value chemicals with impact on modern societies by helping to build the foundations for future circular carbon economies with balanced carbon cycles in materials production, by providing new routes to polymerization processes, by devising new ways to recycle hydrocarbon-based waste, or by making available new pharmaceuticals with new functionalities.