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

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 (Pt₁Pd₁/NCNC) are successfully synthesized using an impregnation-adsorption method. The Pt₁Pd₁/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 Pt₁Pd₁/NCNC are electro-oxidized to acetate ion and CO₂ as the final product, respectively. Pt₁Pd₁/NCNC exhibits long-term stability toward ethanol and methanol oxidation due to the absence of the CO intermediate. Ab initio simulations show that Pt₁Pd₁/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.