Competitive Coordination-Oriented Monodispersed Cobalt Sites on a N-Rich Porous Carbon Microsphere Catalyst for High-Performance Zn−Air Batteries

Metal/nitrogen-doped carbon single-atom catalysts (M−N−C SACs) show excellent catalytic performance with a maximum atom utilization and customizable tunable electronic structure. However, precisely modulating the M−N_x coordination in M−N−C SACs remains a grand challenge. Here, we used a N-rich nucleobase coordination self-assembly strategy to precisely regulate the dispersion of metal atoms by controlling the metal ratio. Meanwhile, the elimination of Zn during pyrolysis produced porous carbon microspheres with a specific surface area of up to 1151 m² g⁻¹, allowing maximum exposure of Co−N₄ sites and facilitating charge transport in the oxygen reduction reaction (ORR) process. Thereby, the monodispersed cobalt sites (Co−N₄) in N-rich (18.49 at%) porous carbon microspheres (CoSA/N−PCMS) displayed excellent ORR activity under alkaline conditions. Simultaneously, the Zn−air battery (ZAB) assembled with CoSA/N−PCMS outperformed Pt/C+RuO₂-based ZABs in terms of power density and capacity, proving that they have good prospects for practical application.