Breaking 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…

• CU
  City University of Hong Kong

  Awards: 9446006, 9228005, 9020003
• NU
  National University of Singapore

  Award: CHI-P2022-04
• NN
  National Natural Science Foundation of China

  Awards: 22388102, 22022504
• ST
  Science, Technology and Innovation Commission of Shenzhen Municipality

  Award: JCYJ20210324103608023
• NS
  National Supercomputing Centre Singapore