Indirect Orbital Hybridization Induced by Nonbonding Interaction at Li‐Intercalated IrO2 Monolayers for Oxygen Evolution Reaction

The development of excellent catalysts with high reactive activity remains a significant challenge for overcoming the sluggish oxygen evolution reaction (OER). Different from other catalysts, herein, a feasible Li intercalation strategy is suggested to regulate the spin‐resolved electronic structures of 2D‐layered IrO 2 nanostructures for improving their reactive activity. When some Li ions are intercalated into the layered IrO 2 materials, the spin splitting at Ir‐5 d orbitals occurs, leading to an obvious reduction in the relative activation energies at OER. The detailed analysis about spin‐resolved electronic structures demonstrates that the intercalated Li ions can provide some 1 s electrons to the O‐2 p orbitals via a weak bonding interaction, for which the electronic occupation at Ir‐5 d orbitals becomes asymmetric, giving rise to a spin polarization. More interestingly, the catalytic activity is enhanced with Li‐intercalation concentration. Herein, a new door is opened to improve OER performance by an intriguing indirect orbital hybridization.