Dizygotic Atomic Platinum and Palladium on Carbon for High‐Performance Ethanol and Methanol Electro‐Oxidation

Abstract Dizygotic‐atom‐site catalysts (DASCs), consisting of multi‐atomic dispersed catalytic centers, perform well in several reactions but have poor electrocatalytic activity toward alcohol electro‐oxidation. In this study, DASCs of atomically dispersed platinum and palladium on nitrogen‐doped carbon nanocages (Pt 1 Pd 1 /NCNC) are successfully synthesized using an impregnation–adsorption method. The Pt 1 Pd 1 /NCNC catalyst has higher mass activity toward ethanol and methanol oxidation than commercial Pt/C and Pd/C. In contrast, Pt or Pd single‐atom catalysts on nitrogen‐doped carbon nanocages are virtually inert. Ethanol and methanol on Pt 1 Pd 1 /NCNC are electro‐oxidized to acetate ion and CO 2 as the final product, respectively. Pt 1 Pd 1 /NCNC exhibits long‐term stability toward ethanol and methanol oxidation due to the absence of the CO intermediate. Ab initio simulations show that Pt 1 Pd 1 /NCNC optimizes the ethanol oxidation pathway thanks to a lower energy barrier and onset potential than individual single Pt or Pd atom catalysts on NCNC. This study opens a new path to developing advanced DASCs for alcohol oxidation.