Ultrahigh-Loaded Fe Single Atoms and Fe₃C Nanoparticle Catalysts as Air Cathodes for High-Performance Zn-Air...

Fe-based materials containing Fe-Nx sites have emerged as promising electrocatalysts in the oxygen reduction reaction (ORR), but they still suffer structural instability which may lead to loss of catalytic activity. Herein, a novel electrocatalyst Fe₃C-FeSA@3DCN with the coexistence of Fe₃C nanoparticles and Fe single atoms (FeSA) in a three-dimensional conductive network (3DCN) is prepared via lattice confinement and defect trapping strategies with an Fe atomic loading of as high as 4.36%. In the ORR process, the limiting current density of Fe₃C-FeSA@3DCN reaches 5.72 mA cm^-2, with an onset potential of 0.926 V and a Tafel slope of 66 mV/decade, showing better catalytic activity and stability than Pt/C catalysts. Notably, its assembled aqueous and solid-state Zn-air batteries (ZABs) achieve peak power densities of 166 and 56 mW cm^-2, respectively, with a long service life of up to 200 h at a current density of 5 mA cm^-2. In addition, the assembled ZAB can provide a constant voltage on activated carbon electrodes to perform capacitive deionization to adsorb different ions. The importance of the Fe species active sites generated by Fe₃C and FeSA in the material for ORR activity to boost the electron transfer and mass transfer is demonstrated by a simple selective poisoning experiment.