Atomically Dispersed Mn within Carbon Frameworks as High-Performance Oxygen Reduction Electrocatalysts for Zinc-Air Battery

Manganese (Mn)-based catalysts are generally not active for the oxygen reduction reaction (ORR) under alkaline conditions. Herein, a Mn-SA electrocatalyst consisted of atomically dispersed pyridinic-N-coordinated Mn atoms within carbon frameworks was prepared. The electrocatalyst exhibited excellent performance for ORR (E-1/2 = 0.87 V) and zinc-air batteries under alkaline conditions, which is superior to that of most Mn-based catalysts and the commercial Pt/C catalyst. Density functional theory (DFT) calculations reveal that the nearest coordination environment can tailor the intrinsic catalytic activity of Mn centers via turning their electronic structure. The high activity of the pyridinic-N-coordinated Mn configuration is attributed to the modest adsorption strength for ORR intermediates and the reasonable position of the d-band center, which boost the ORR process.