Coupling Magnetic Single‐Crystal Co₂Mo₃O₈ with Ultrathin Nitrogen‐Rich Carbon Layer for Oxygen Evolution Reaction

Transition-metal oxides as electrocatalysts for the oxygen evolution reaction (OER) provide a promising route to face the energy and environmental crisis issues. Although palmeirite oxide A₂ Mo₃ O₈ as OER catalyst has been explored, the correlation between its active sites (tetrahedral or octahedral) and OER performance has been elusive. Now, magnetic Co₂ Mo₃ O₈ @NC-800 composed of highly crystallized Co₂ Mo₃ O₈ nanosheets and ultrathin N-rich carbon layer is shown to be an efficient OER catalyst. The catalyst exhibits favorable performance with an overpotential of 331 mV@10 mA cm⁻² and 422 mV@40 mA cm⁻² , and a full water-splitting electrolyzer with it as anode catalyst shows a cell voltage of 1.67 V@10 mA cm⁻² in alkaline. Combined HAADFSTEM, magnetic, and computational results show that factors influencing the OER performance can be attributed to the tetrahedral Co sites (high spin, t₂ ³ e⁴ ), which improve the OER kinetics of rate-determining step to form *OOH.