Boosting the Catalytic Activity of Nitrogen Sites by Spin Polarization Engineering for Oxygen Reduction and Wide‐Temperature Ranged Quasi‐Solid Zn–Air Batteries

Abstract The oxygen reduction reaction (ORR) is a crucial cathode reaction for developing quasi‐solid zinc–air batteries (QZABs) with high energy density. However, the activity and stability of catalysts under extreme conditions have not been fully explore. Herein, a series of systematic experiments and theoretical calculations have been conducted to investigate the potential of introducing Fe x Co y into nitrogen (N)‐doped porous carbon (NPC) via one‐step pyrolysis to form a core–shell structure that can effectively enhance the activity of the catalysts, particularly at low temperatures. Due to the difference in the work function of 5.12, 5.11, and 5.06 eV, the spin‐polarized charge is transferred to the pyridinic‐N site on the surface under the charge transfer. Consequently, the pyridinic‐N site on the surface exhibits varying degrees of magnetic moment 0.024 µ B , which is crucial for forming OOH* and enhances ORR activity. The Fe 5 Co 5 @NPC catalyst is evaluated for QZABs at −40 °C and achieved a power density of up to 117.6 mW cm −2 , which is only 18.7% lower than normal temperature, and a cycle life of up to 300 h. This study provides a means to realize the design of QZABs catalysts in extreme environments and explore their application potential.