Homogeneous Oxygen Reduction Electrocatalysis via Decoupling Active Sites from Carbon Supports

Conventional nanocarbon-supported metal single-atom catalysts (SACs) as the heterogeneous electrocatalyst system of coupled active sites with carbon support (CAS) suffer from serious uncontrollability, inhomogeneity, and insufficient utilization of active configurations as well as limited reaction kinetics. Herein, a novel homogeneous electrocatalyst system via decoupling the active sites from the carbon support (DAS) was proposed. By incorporating a soluble macrocycle with TM–N4 centers into an electrolyte while loading carbon supports on the current collector, the developed novel DAS-typed oxygen reduction reaction (ORR) electrocatalytic system demonstrated huge advantages of multiscale regulations from surface properties of carbon supports to molecular configurations of TM–N4 sites and fast interfacial charge transfer kinetics with decreased reaction energy barrier, resulting in superior ORR activity for Zn-air battery application. This novel catalyst design principle will promote the development of advanced catalyst systems for energy conversion applications.