Magnetic Field Modulated Intrinsic Charge and Spin Ordering in Ferromagnetic Electrocatalysts for Rechargeable Zn–Air Battery

Abstract Magnetic field‐enhanced electrocatalytic activity has recently emerged as an effective strategy for electrocatalytic reactions. However, modulating the electrical behavior and spin ordering in real‐time using magnetic field during the electrocatalytic process remains challenging. Herein, based on the coexistence of room‐temperature ferromagnetic and magnetoresistance (MR) properties in La_1−xSr_xMnO₃, it demonstrates that in addition to spin polarization, the negative MR effect contributes significantly to the enhancement of the oxygen evolution reaction (OER) owing to the considerable MR value (−7.32% for La_0.8Sr_0.2MnO₃ at 1.0 T). Accordingly, a lessened OER overpotential of ≈120 mV (at 10 mA cm⁻²) and a reduced charge‐transfer resistance are observed in La_0.8Sr_0.2MnO₃ under a magnetic field of 1.0 T. Additionally, the power density of self‐assembled Zn–air battery (ZnAB) based on La_0.8Sr_0.2MnO₃ improves by 5.9 times under 1.0 T. Calculation results reveal that spin alignment can induce more unoccupied electronic states near the Fermi level, decrease the energy level of the Mn d‐band center, and significantly reduce the O^* formation barrier to enhance the OER activity of Sr‐doped LaMnO₃. Thus, the in situ regulation of charge and spin ordering by magnetic field offers a deeper understanding for designing high‐performance ZnABs.