Decoupling of Spin and Non‐Spin Effects From Electronic Structure Modulation for Oxygen Electrocatalysis

. While the modulation strategies (built-in electric fields, built-in magnetic fields, crystal fields and ligand fields) advance electronic structure engineering for catalyst design. Nevertheless, they inevitably co-regulate spin effects (spin state/polarization) and non-spin effects (d-band center shifts, valence tuning, etc.), making it difficult to distinguish the individual contributions to catalytic performance. This review systematically distinguishes the influence of spin/non-spin factors in electronic structure-modulated OER/ORR, aiming to clarify their regulatory mechanisms, contribution ratios, and synergistic effects. Statistical analyses indicate that spin-related and non-spin-related effects exhibit comparable importance, with synergistic regulation yielding superior OER performance. Further analyzing their distinct roles in dynamics (adsorption/desorption) and kinetics (spin flip/selective electron transfer), this work proposes a deeply decoupling approach to disentangle these effects, providing new perspectives for rational design of spin-controlled electrocatalysts and optimizing catalytic performance beyond traditional constraints.