Reprogramming the reactivity of main-group compounds for capturing and activating methane and dinitrogen

The activation of chemical bonds is fundamental to every chemical transformation. While reactions mediated by transition-metal catalysts are known for more than a century, the last decade witnessed spectacular developments in the emerging area of catalysis mediated by non-metallic species. Among these new chemical entities made from earth-abundant and inexpensive main-group elements, Lewis acid-base pairs and bifunctional element/ligand systems mimicking the behavior of transition-metals rapidly revolutionized the activation modes of chemical bonds. In the project B-yond, I will establish new molecular engineering strategies and develop unprecedented main-group catalysts embedded in cage-shaped and curved molecular scaffolds. Ground-breaking molecules escaping the established structural theories will become the initial focus of my project, including the creation of non-planar B, Al, C and Si centered Lewis superacids with unmatched reactivities. I will push the frontiers of knowledge of chemical bonding by exploring unusual boron-elements bonding situations and advance the design of main-group catalysts beyond the state-of-the-art. Unprecedented C-H bond functionalization processes will be developed and exploited for hydrocarbons transformation through the concept of “low reorganization energy catalysts”. The activation of dinitrogen with unique main-group superacids and bases will finally be tackled, a pioneering step toward the uncharted territory of catalytic N2 activation and conversion without transition-metal complexes. These goals will be accomplished through a multidisciplinary approach built on my expertise in mechanistic investigations, spectroscopic and kinetics methods, organometallic and main group chemistry. The project B-yond will deliver extraordinary solutions for chemists to reach new chemical reactivities beyond the actual limits and will inspire scientists to develop innovative sustainable and cost-effective chemical processes.