Reconstruction of pH-universal atomic FeNC catalysts towards oxygen reduction reaction

[Display omitted] •The three-dimensional hierarchically architectural FeNC catalyst was prepared through silicon template.•The ammonia-assisted secondary pyrolysis boosted the density of FeNx active sites.•The FeNC catalyst delivers outstanding ORR activity in pH-universal electrolyte. Constructing of single atom catalysts that can stably exist in various energy conversion and storage devices is still in its infancy. Herein, a geometrically optimized three-dimensional hierarchically architectural single atomic FeNC catalyst with fast mass transport and electron transfer is rationally developed by post-molecule pyrolysis assisted with silicon template and reconstructs by ammonia treating. The ammonia-assisted secondary pyrolysis not only compensates for the volatilization of nitrogen species contained in organic precursors but also optimizes the surface structure of FeNC catalyst, thus increasing the content of pyridinic nitrogen and boosting the density of active sites (FeNx) in FeNC samples. In addition, the pyridinic nitrogen adjusts the electronic distribution in Fe 3d active center and promotes the catalytic performances. Therefore, this hollow spherical atomically dispersed FeNC catalyst delivers outstanding oxygen reduction reaction (ORR) activity in pH-universal electrolyte and surpasses the most reported values.