Chemical Ordering Command Dynamic Reconstruction for Enhanced Water Oxidation.

Dynamic surface reconstruction fundamentally dictates the active state of electrocatalysts. However, the lack of mastery over reconstruction kinetics typically imposes a trade-off between high activity and long-term stability. Here, we demonstrate that the degree of chemical ordering (long-range atomic site occupancy) deterministically governs the evolution of alloy surfaces under operating conditions. In this design, the chemical ordering acts as a structural template that commands the reconstruction trajectory. During anodic dealloying, the ordered lattice facilitates a controlled, mild pre-oxidation. This process generates high-valence Fe/Co/Ni sites that trigger a well-balanced, synergistic adsorbate evolution mechanism (AEM)/lattice oxygen mechanism (LOM) dual pathway. Unlike disordered counterparts that suffer from severe deterioration, the thermodynamically stable intermetallic core prevents excessive metal dissolution, reducing elemental leaching by 97.2%, guiding the formation of a homogeneous active reconstruction layer. As a result, the catalyst achieves an overpotential of only 335 mV at 1 A cm-2 and maintains exceptional stability for over 1000 h. Even under industrial conditions (6 M KOH, 353 K), it reaches 3 A cm-2 at only 1.50 V. This work establishes chemical ordering as a predictive parameter to govern dynamic reconstruction, offering a robust framework for designing self-adaptive catalysts that harmonize extreme activity with industrial-grade durability.