Atomically Defined Nanopropeller FeCoSe(PhPNTol): Functional Model for the Electronic Metal-Support Interaction Effect and High Catalytic Activity for Carbodiimide Formation.

Atomically defined interfaces that maximize the density of active sites and harness the electronic metal-support interaction are desirable to facilitate challenging multielectron transformations, but their synthesis remains a considerable challenge. We report the rational synthesis of the atomically defined metal chalcogenide nanopropeller FeCoSeL (L = PhPNTol) featuring three Fe edge sites, and its ensuing catalytic activity for carbodiimide formation. The complex interaction between the Fe edges and CoSe support, including the interplay between oxidation state, substrate coordination, and metal-support interaction, is probed in detail using chemical and electrochemical methods, extensive single crystal X-ray diffraction, and electronic absorption and Mössbauer spectroscopy.