Spin-related electronic state coupling between surface strain and magnetic dopants in free-standing IrO2 monolayers

Abstract

The acidic oxygen evolution reaction (OER) strongly depends on the spin-related electronic configuration of metal sites at catalyst surfaces, which can directly affect the structural stability and catalytic activity. Recently, layered two-dimensional IrO2 nanostructures with typical metallic characteristic have been successfully realized. However, the electronic state coupling between magnetic dopants and structural strain still need be understood as they can effectively enhance the catalytic activity. Herein, a series of magnetic dopants are intentionally implanted into the IrO2 monolayers with different structural deformations in order to trigger the spin-related electronic reconfigurations for regulating the orbital interactions and charge transfer with reactants. Accordingly, the acidic OER performance is obviously enhanced because doped magnetic dopants with half-filled 3d orbitals can donate some valence electrons to the intermediates more easily, leading to a lower activation energy. This work provides a new insight into designing catalysts for acidic OER by particular electronic state coupling.