Slow Synthesis Methodology‐Directed Immiscible Octahedral PdxRh1−x Dual‐Atom‐Site Catalysts for Superior Three‐Way Catalytic Activities over Rh

This study provided an effective strategy to construct dual-atom sites by solid-solution alloying. A slow synthesis methodology was established for the solid-solution preparations as dual-atom-site catalysts. The atomic-level homogeneous Pdx Rh1-x dual-atom-site catalysts were successfully synthesized over the whole composition range, as evidenced by X-ray powder diffraction and scanning transmission electron microscope energy-dispersive X-ray spectroscopy mapping measurements. The challenging morphology formation in the immiscible alloys was achieved by an energy-controlling process as the octahedral Rh-rich alloys. The Pd0.3 Rh0.7 dual-atom-site catalyst had unique surface states to activate the key reactants of CO and NO in the complex three-way catalytic reactions, and it performed significantly better than pure Rh.