Regulating the Spin Polarization of NiFe Layered Double Hydroxide for the Enhanced Oxygen Evolution Reaction

The oxygen evolution reaction (OER) is an electrochemical process that involves the spin-dependent conversion of singlet OH^–/H₂O to triplet O₂. However, the sluggish dynamics associated with this reaction severely limits its efficiency in electrochemical water splitting. Fortunately, the utilization of a magnetic field can significantly enhance the spin selectivity and accelerate reaction kinetics. Herein, we report a unique strategy to regulate the spin polarization of NiFe layered double hydroxide (NiFe-LDH) by harnessing an internal magnetic field induced by a built-in magnetic core. The exchange bias effect between the magnetic core and NiFe-LDH can selectively remove electrons with opposite magnetic moments, thereby reducing magnetoresistances and minimizing spin scattering during electron transport. Benefiting from this bias effect, the obtained catalyst exhibits excellent OER performance with a low overpotential of 196 mV at a current density of 30 mA cm^–2. Furthermore, density functional theory (DFT) calculations further confirm that the exchange bias effect can increase the hybrid strength of Fe-3d and O-2p orbitals while decreasing the adsorption energy of the reactant intermediates, thus accelerating the generation of paramagnetic oxygen.