A Vacuum Vapor Deposition Strategy to Fe Single-Atom Catalysts with Densely Active Sites for High-Performance Zn-Air Battery.

Abstract

Iron single-atom catalysts (SACs) have garnered increasing attention as highly efficient catalysts for the oxygen reduction reaction (ORR), yet their performance in practical devices remains suboptimal due to the low density of accessible active sites. Anchoring iron single atoms on 2D support is a promising way to increase the accessible active sites but remains difficult attributing to the high aggregation tendency of iron atoms on the 2D support. Herein, a vacuum vapor deposition strategy is presented to fabricate an iron SAC supported on ultrathin N-doped carbon nanosheets with densely active sites (FeSAs-UNCNS). Experimental analyses confirm that the FeSAs-UNCNS achieves densely accessible active sites (1.11×1020sitesg-1) in the configuration of Fe─N4O. Consequently, the half-wave potential of FeSAs-UNCNS in 0.1m KOH reaches a remarkable value of 0.951V versus RHE. Moreover, when employed as the cathode of various kinds of Zn-air batteries, FeSAs-UNCNS exhibits boosting performances by achieving a maximum power density of 306mWcm-2 and long cycle life (>180h) at room temperature, surpassing both Pt/C and reported SACs. Further investigations reveal that FeSAs-UNCNS facilitates the mass and charge transfer during catalysis and the atomic configuration favors the desorption of *OH kinetically.