Kagome-Lattice Magnetic Catalysts: Electric Potential and Magnetic Field Dual Modulation for Enhanced Oxygen Reduction Reaction

Herein, we employed density functional theory (DFT) calculations and Monte Carlo simulations to investigate two-dimensional (2D) Kagome-lattice TM 3 (CN 3 ) 2 metal–organic frameworks (MOFs), probing the effect of magnetic states on electrocatalytic oxygen reduction reaction (ORR) under dual conditions of electric potential and magnetic fields. Specifically, transition metals (TM) substitution governs magnetic axis reorientation (out-of-plane ↔ in-plane) and Curie temperature modulation, with magnetic orbital projections revealing mechanistic insights. The ferromagnetic (FM) Fe 3 (CN 3 ) 2 exhibits efficient 2e − ORR (0.03 V overpotential, 0.93 V/RHE onset). For Fe 3 (CN 3 ) 2 (near-room-temperature phase transitions), elevating temperature or applying potential switches the ORR pathway from 2e − (FM state) to 4e − (antiferromagnetic, AFM). Monte Carlo simulations further show that, once the magnetic state is established by the applied electric potential, the external magnetic field can tune the relative stability among different magnetic configurations. In this way, electric potential and magnetic field play distinct but complementary roles in regulating the catalytic behavior.