Regulating Magnetic Behavior of Fe in Hematene by Defects to Improve Oxygen Evolution Reaction

Two-dimensional hematene is earth-abundant and exhibits easy modulation with unique electronic properties, suggesting a promising role as an electrocatalyst for oxygen evolution reaction (OER). In this Letter, we propose a strategy to regulate the magnetic behavior of Fe atoms in hematene by introducing structural defects to enhance its OER activity. Hematene is proved to be thermodynamically stable at electrolyte pH values ≥3 under the OER working potential according to the Pourbaix diagram. Among all the defective structures, the most stable DV_Fe1-O defect exhibits superior OER activity, which originates from the unique spin state of the active Fe atom. We further propose a novel descriptor of the magnetic moment difference on active Fe to efficiently evaluate the OER activity. We believe that our strategy of combining the defect modulation in the geometric structure and spin-state control in the electronic configuration could provide a guideline to design highly active Fe-based electrocatalysts.