Chalil Oglou, RamadanUlusoy Ghobadi, Türkan GamzeHegner, F. S. .Galán-Mascarós, J. R.López, NÖzbay, EkmelKaradaş, Ferdi2024-03-132024-03-132023-10-261433-7851https://hdl.handle.net/11693/114665Electrocatalytic processes involving the oxygen evolution reaction (OER) present a kinetic bottleneck due to the existence of linear-scaling relationships, which bind the energies of the different intermediates in the mechanism limiting optimization. Here, we offer a way to break these scaling relationships and enhance the electrocatalytic activity of a Co−Fe Prussian blue modified electrode in OER by applying external stimuli. Improvements of ≈11 % and ≈57 % were achieved under magnetic field (0.2 T) and light irradiation (100 mW cm−2), respectively, when working at fixed overpotential, η=0.6 V at pH 7. The observed enhancements strongly tie in with the intermetallic charge transfer (IMCT) intensity between Fe and Co sites. Density Functional Theory simulations suggest that tuning the IMCT can lead to a change of the OER mechanism to an external stimuli-sensitive spin crossover-based pathway, which opens the way for switchable electrocatalytic devices.enDensity funcional theoryElectrocatalysisExternal stimuliIntermetallic charge transferPrussian blue analoguesArticle10.1002/anie.2023086471521-3773