Spin State Modulation in Cr₂VC₂-MXene Promotes Efficient C-N Coupling for Direct Electrosynthesis of Urea From CO₂...

Urea has gained considerable interest as a hydrogen carrier for safe, sustainable, and long-term energy storage. In this work, magnetic Cr₂VC₂-MXene is shown to facilitate efficient C-N coupling during the direct electrocatalytic synthesis of urea from CO₂ and N₂. Our findings reveal that Cr₂VC₂-MXene possesses a ferromagnetic ground state and exhibits outstanding catalytic activity and stability throughout urea formation. The transition metal layer on the catalyst surface supplies additional charge to both CO₂ and N₂ molecules by populating the antibonding orbitals of their lowest unoccupied molecular orbitals (LUMOs). The incorporation of magnetism promotes the excitation of more electrons from bonding to antibonding states in the C─O bonds, thereby weakening these bonds and enhancing CO₂ activation. This study offers theoretical insights into the mechanism of magnetic regulation in catalysis, providing a valuable reference for future research on urea synthesis.