Novel (Pt‐O_x)‐(Co‐O_y) Nonbonding Active Structures on Defective Carbon from Oxygen‐Rich Coal Tar Pitch for Efficient HER and ORR

Abstract Atomic‐scale utilization and coordination structure of Pt electrocatalyst is extremely crucial to decrease loading mass and maximize activity for hydrogen evolution reactions (HERs) and oxygen reduction reactions (ORRs). A novel atomic‐scale (Pt‐O_x)‐(Co‐O_y) nonbonding active structure is designed and constructed by anchoring Pt single atoms and Co atomic clusters on the defective carbon derived from oxygen‐rich coal tar pitch (CTP). The Pt loading mass is extremely low and only 0.56 wt%. A new nonbonding interaction phenomenon between Pt‐O_x and Co‐O_y is found and confirmed based on X‐ray absorption spectroscopy and density functional theory calculations. Based on the (Pt‐O_x)‐(Co‐O_y) nonbonding active structure, surface chemical field coupling with electrocatalysis for the HER and ORR is confirmed. It is found that the (Pt‐O_x)‐(Co‐O_y) nonbonding active structure exhibits high mass activities of 64.4 A cm⁻² mg_Pt⁻¹ (at an overpotential of 100 mV) and 7.2 A cm⁻² mg_Pt⁻¹ (at 0.8 V vs reversible hydrogen electrode) for the HER and ORR, respectively. The values are 6.5 and 11.6 times as much as those of commercial 20% Pt/C. The work provides innovative insight to design and understand efficient active sites of atomic‐scale Pt on oxygen‐rich CTP‐derived carbon supports for electrocatalysis.