John Anderson, University of Chicago

3:45 pm Zoom

"Leveraging Exotic Electronic Structures in Transition Metal Molecules and Materials"

Disparate fields including catalysis, biology, and materials chemistry all rely upon transition metals. Decades of research have yielded deep insights into how the electronic structure of metal centers dictates their properties and reactivity. However, transforming these deep insights into tractable strategies for new transformations or functionality remains an outstanding challenge. I will present our group’s progress at not only uncovering, but leveraging, new electronic structure paradigms in this area. I will show how an unusual Co–O bond has triggered a reconsideration of classic dogmas in transition metal oxo mediated CPET reactions. We show that semiclassical transition state theory contributions can dictate selectivity even in nonadiabatic CPET reactions. Furthermore, generation of even more oxidized Co–O cores results in hydroxylation with rates comparable to the fastest biological systems. I will then cover our efforts in expanding proton storage and electron delocalization across conjugated ligand frameworks. This strategy enables new pathways for the activation of oxygen and also leads to highly efficient reductive and aerobic catalysis. Finally, I will show how expanding electron delocalization across even longer length scales enables the tuning of macroscopic material properties. Unusual diradical electronic structures offer exciting possibilities for near-IR emission, qubits, and new bulk properties even in amorphous materials. While varying in length and localization from a single bonding interaction to macroscopic charge transport, all these advances are rooted in understanding and utilizing unusual electronic structures of transition metal centers and their coordination spheres.

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Oct 4