Controlling Multiple Active Sites on Pd−CeO 2 for Sequential C−C Cross‐coupling and Alcohol Oxidation in One Reaction System

Ceria (CeO 2 )‐supported metal catalysts have been widely utilized for various single‐step chemical transformations. However, using such catalysts for a multistep organic reaction in one reaction system has rarely been achieved. Here, we investigate multiple active sites on Pd−CeO 2 catalysts and optimize them for a multistep reaction of C−C cross‐coupling and alcohol oxidation. Atomic‐level imaging and spectroscopic studies reveal that metallic Pd 0 and Pd−CeO 2 interface are active sites on Pd−CeO 2 for C−C cross‐coupling and oxidation, respectively. These active sites are controlled under the structural evolution of Pd−CeO 2 during reductive heat‐treatments. Accordingly, we found that optimally reduced Pd−CeO 2 catalysts containing ∼1.5 nm‐sized Pd nanoclusters with both sites in balance are ideal for multistep chemical transformations in one reaction system. Our strategy to design supported metal catalysts leads to one‐pot sequential synthetic protocols for pharmaceutical building blocks.