Metal-ligand complexation offers the opportunity to both stabilize and chemically tune single transition metal atoms on a support surface. This offers a solution to grand challenges in heterogeneous catalysis to achieve high levels of selectivity by controlling the chemical uniformity of metal catalyst sites at surfaces. Here, we present fundamental research on model surfaces in ultra-high vacuum environments to demonstrate design concepts in metal-ligand coordination at surfaces. The metal centers are stabilized in extended, ordered metal-organic complexes that self-assemble through an on-surface redox process and are characterized by X-ray photoelectron spectroscopy, scanning tunneling microscopy, and high-resolution electron energy loss spectroscopy. We also present work that applies those design concepts to high surface area oxide support surfaces that show excellent activity and selectivity as heterogeneous catalysts. These systems are shown to be active for the catalysis of hydrosilylation reactions at a level that is competitive with current homogeneous catalysts. They also show excellent activity for hydrogenation in flow reactor experiment.

Metal-ligand complexation at model surfaces and on high-surface-area oxide supports

ACS Spring Meeting 2021

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