Light‐Driven Surface Lattice Oxygen Activation in Oxygen Evolution

ABSTRACT The oxygen evolution reaction (OER) remains a key bottleneck in sustainable hydrogen production and energy conversion. Conventional pathways such as the adsorbate evolution mechanism (AEM) and lattice oxygen oxidation mechanism (LOM) both suffer from electron‐transfer inefficiencies at their potential‐determining steps ( * OOH formation in AEM and deprotonation in LOM) and structural instability (metal oxidation in AEM and oxygen‐vacancy accumulation in LOM). As a result, a unified mechanism that simultaneously overcomes these kinetic limitations and structural degradation processes remains absent. Here, we present a light‐driven surface lattice oxygen activation mechanism (LSOM) that synergizes photoexcitation and electrocatalysis to activate surface lattice oxygen into high‐energy non‐bonding orbitals, enabling their direct participation in O─O bond formation. This strategy circumvents the potential‐determining steps inherent to both AEM and LOM, while preserving metal oxidation states and lattice structural integrity. Experimental validation confirms remarkable enhancements in electrocatalytic activity and stability, outperforming conventional OER systems. By unifying catalytic efficiency with structural durability, the LSOM redefines the design principles for OER and establishes a universal framework for robust energy conversion technologies.