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Updated: Aug 6, 2026

Multiscale Sampling of a Heterogeneous Water/Metal Catalyst Interface using Density Functional Theory and Force-Field Molecular Dynamics
Published on: April 12, 2019
Chemical Ordering Command Dynamic Reconstruction for Enhanced Water Oxidation
Yiyuan Yang1,2,3, Chengkai Jin4, Zhe Jia1
1School of Materials Science and Engineering, Southeast University, Nanjing, China.
Abstract:
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.
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