Engineering the Local Atomic Environments of Te‐Modulated Fe Single‐Atom Catalysts for High‐Efficiency O₂ Reduction

Abstract Atomically dispersed metal‐nitrogen‐carbon materials (AD‐MNCs) are considered the most promising non‐precious catalysts for the oxygen reduction reaction (ORR), but it remains a major challenge for simultaneously achieving high intrinsic activity, fast mass transport, and effective utilization of the active sites within a single catalyst. Here, an AD‐MNCs consisting of defect‐rich Fe‐N₃ sites dispersed with axially coordinated Te atoms on porous carbon frameworks (Fe₁Te₁‐900) is designed. The local charge densities and energy band structures of the neighboring Fe and Te atoms in FeN₃‐Te are rearranged to facilitate the catalytic conversion of the O‐intermediates. Meanwhile, the negative shift of the d‐band center in FeN₃‐Te reduces the energy barrier limit for effective desorption of the final OH^* intermediate. In the electrochemical evaluation, Fe₁Te₁‐900 presents a more positive onset potential and half‐wave potentials of 1.03 and 0.89 V versus the reversible hydrogen electrode, respectively. Furthermore, the liquid zinc‐air batteries assembled with Fe₁Te₁‐900 exhibited excellent performances compared to commercial Pt/C. This work opens up new ideas for the development of high‐performance ORR electrocatalysts for applications in various energy conversion and storage technologies.