Creating Spin Channels in SrCoO ₃ through Trigonal‐to‐Cubic Structural Transformation for Enhanced Oxygen Evolution/Reduction Reactions

Abstract Oxygen evolution and reduction reactions (OER and ORR) play crucial roles in energy conversion processes such as water splitting and air batteries, where spin dynamics inherently influence their efficiency. However, the specific contribution of spin has yet to be fully understood. In this study, we intentionally introduce a spin channel through the transformation of trigonal antiferromagnetic SrCoO 2.5 into cubic ferromagnetic SrCoO 3 , aiming to deepen our understanding of spin dynamics in catalytic reactions. Based on the results from spherical‐aberration‐corrected microscopy, synchrotron absorption spectra, magnetic characterizations, and density functional theory calculations, it is revealed that surface electron transfer is predominantly governed by local geometric structures, while the presence of the spin channel significantly enhances the bulk transport of spin‐polarized electrons, particularly under high current densities where surface electron transfer is no longer the limiting factor. The overpotential for OER is reduced by at least 70 mV at 150 mA cm −2 due to the enhanced conductivity from spin‐polarized electrons facilitated by spin channels, with an expectation of even more significant reductions at higher current densities. This work provides a clearer picture of the role of spin in oxygen‐involved electrocatalysis, providing critical insights for the design of more efficient catalytic systems in practical applications.