Double Riveting and Steric Hindrance Strategy for Ultrahigh‐Loading Atomically Dispersed Iron Catalysts Toward Oxygen Reduction

Abstract Atomically dispersed iron on nitrogen doped carbon displays high intrinsic activity toward oxygen reduction reaction, and has been identified as an attractive candidate to precious platinum catalysts. However, the loading of atomic iron sites is generally limited to below 4 wt% due to the undesired formation of iron‐related particles at higher contents. Herein, this work overcomes this limit by a double riveting and steric hindrance strategy to achieve monodispersed iron with a high‐loading of 12.8 wt%. Systematic study reveals that chemical riveting of atomic iron in ZIF‐8 framework, chelation of Fe ions with interconfined 1,4‐phenylenebisboronic, and physical hindrance are essential to obtain high‐loading monodispersed Fe moieties. Resultantly, designed Fe‐N‐C‐PDBA exhibits superior catalytic activity and excellent stability over commercial platinum catalysts toward oxygen reduction reaction in both half‐cells and zinc‐air fuel cells (ZAFCs). This provides an avenue for developing high‐loading single‐atom catalysts (SACs) for energy devices.