Single-atom catalysts offer the potential to transform heterogeneous catalysis by offering highly uniform and specifically tuned metal centers that can achieve high selectivity and catalyze new reactions. Metal-ligand complexation offers a strategy to isolate, stabilize, and chemically tune single transition metal atoms on a support surface. These ligand-coordinated supported catalysts have been shown to be effective for a variety of reactions. Here, we examine the significant roles of the coordinating ligands and of the oxide support on catalyst structure, activity, and stability. Defect sites on the support have a strong influence on the state of the metal centers and show a significant impact on reaction activity. We also see strong influences due to changing functional group substituents in the ligands or by changing the ligand to metal loading ratio on the catalyst. By loading the metal and ligand directly on the oxide support, it is possible to maintain a close contact of the metal to the oxide, which can facilitate spillover during the reaction. These systems are shown to be active for the catalysis of hydrosilylation reactions in solution and for hydrogenation in flow reactor experiments.

Tuning and stabilization of metal-ligand single-atom catalysts at surfaces by ligand design and support treatment

ACS Spring 2022

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