A Bimetallic Zn/Fe Polyphthalocyanine‐Derived Single‐Atom Fe‐N4 Catalytic Site:A Superior Trifunctional Catalyst for Overall Water Splitting and Zn–Air Batteries

Abstract Developing an efficient single‐atom material (SAM) synthesis and exploring the energy‐related catalytic reaction are important but still challenging. A polymerization–pyrolysis–evaporation (PPE) strategy was developed to synthesize N‐doped porous carbon (NPC) with anchored atomically dispersed Fe‐N 4 catalytic sites. This material was derived from predesigned bimetallic Zn/Fe polyphthalocyanine. Experiments and calculations demonstrate the formed Fe‐N 4 site exhibits superior trifunctional electrocatalytic performance for oxygen reduction, oxygen evolution, and hydrogen evolution reactions. In overall water splitting and rechargeable Zn–air battery devices containing the Fe‐N 4 SAs/NPC catalyst, it exhibits high efficiency and extraordinary stability. This current PPE method is a general strategy for preparing M SAs/NPC (M=Co, Ni, Mn), bringing new perspectives for designing various SAMs for catalytic application.