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To reach a long term viable green hydrogen economy, rational design of activeoxygen evolution reaction (OER) catalysts is critical. An important hurdle inthis reaction originates from the fact that the reactants are singletmolecules, whereas the oxygen molecule has a triplet ground state with parallelspin alignment, implying that magnetic order in the catalyst is essential.Accordingly, multiple experimentalists reported a positive effect of externalmagnetic fields on OER activity of ferromagnetic catalysts. However, it remainsa challenge to investigate the influence of the intrinsic magnetic order oncatalytic activity. Here, we tuned the intrinsic magnetic order of epitaxialLa$_{0.67}$Sr$_{0.33}$MnO$_{3}$ thin film model catalysts from ferro- toparamagnetic by changing the temperature in-situ during water electrolysis.Using this strategy, we show that ferromagnetic ordering below the Curietemperature enhances OER activity. Moreover, we show a slight current densityenhancement upon application of an external magnetic field and find that thedependence of magnetic field direction correlates with the magnetic anisotropyin the catalyst film. Our work thus suggests that both the intrinsic magneticorder in La$_{0.67}$Sr$_{0.33}$MnO$_{3}$ films and magnetic domain alignmentincrease their catalytic activity. We observe no long-range magnetic order atthe catalytic surface, implying that the OER enhancement is connected to themagnetic order of the bulk catalyst. Combining the effects found with existingliterature, we propose a unifying picture for the spin-polarized enhancement inmagnetic oxide catalysts.

Beyond domain alignment: Revealing the effect of intrinsic magnetic order on electrochemical water splitting