biostudies-literatureZhang ZCity University of Hong Kong (CityU)National University of Singapore (NUS)1301https://www.ebi.ac.uk/biostudies/studies/S-EPMC11790916biostudies-literatureUnknown16(1)The universal linear scaling relationships between the adsorption energies of reactive intermediates limit the performance of catalysts in multi-step catalytic reactions. Here, we show how these scaling relationships can be circumvented in electrochemical oxygen evolution reaction by dynamic structural regulation of active sites. We construct a model Ni-Fe₂ molecular catalyst via in situ electrochemical activation, which is able to deliver a notable intrinsic oxygen evolution reaction activity. Theoretical calculations and electrokinetic studies reveal that the dynamic evolution of Ni-adsorbate coordination driven by intramolecular proton transfer can effectively alter the electronic structure of the adjacent Fe active centre during the catalytic cycle. This dynamic dual-site coNature communicationsBreaking linear scaling relationships in oxygen evolution via dynamic structural regulation of active sites.PMC11790916CHI-P2022-049020003Bin Yang HChen PZhang ZChen ZWang YGLiu BChi XXi SYu XZhao HZhao XfalseBreaking linear scaling relationships in oxygen evolution via dynamic structural regulation of active sites.The universal linear scaling relationships between the adsorption energies of reactive intermediates limit the performance of catalysts in multi-step catalytic reactions. Here, we show how these scaling relationships can be circumvented in electrochemical oxygen evolution reaction by dynamic structural regulation of active sites. We construct a model Ni-Fe₂ molecular catalyst via in situ electrochemical activation, which is able to deliver a notable intrinsic oxygen evolution reaction activity. Theoretical calculations and electrokinetic studies reveal that the dynamic evolution of Ni-adsorbate coordination driven by intramolecular proton transfer can effectively alter the electronic structure of the adjacent Fe active centre during the catalytic cycle. This dynamic dual-site co2025-01-01T00:00:00Z2025 Feb2025-04-04T01:02:18.32Z2025-04-04T01:02:18.32ZS-EPMC117909163990089310.1038/s41467-024-55150-9