Electrocatalytic Oxygen Reduction to Hydrogen Peroxide on Graphdiyne-Based Single-Atom Catalysts: First-Principles Studies

The electrocatalytic oxygen reduction reaction (2e− ORR) via a two-electron process is promising pathway for the production of hydrogen peroxide (H2O2). Here, we systematically investigated 2e− ORR on graphdiyne (GDY) supported single transition metal atoms (TM1@GDY) using density functional theory (DFT) calculations. Among 23 TM1@GDY catalysts, Pt1@GDY showed best performance H2O2 product with an overpotential as low 0.15 V. electronic structure analysis, one hand, elucidates that electron transfer between and adsorbed O2 facilitates activation O2, and, other reveals high activity lies in electrons from filled Pt-3d orbitals to 2p antibonding OOH*, which effectively activates O–O bond. This work provides insights design efficient electrocatalysts generation.