Spin State Modulation in Cr 2 VC 2 ‐MXene Promotes Efficient C–N Coupling for Direct Electrosynthesis of Urea From CO 2 Neng Li, Bin Liu, Zhongyong Zhang, Yucheng Feng, Ruiyang Ma, Yufei Yang, Xing Zhou, Shifeng Wang
Urea has gained considerable interest as a hydrogen carrier for safe, sustainable, and long‐term energy storage. In this work, magnetic Cr 2 VC 2 ‐MXene is shown to facilitate efficient C–N coupling during the direct electrocatalytic synthesis of urea from CO 2 and N 2 . Our findings reveal that Cr 2 VC 2 ‐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 CO 2 and N 2 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 CO 2 activation. This study offers theoretical insights into the mechanism of magnetic regulation in catalysis, providing a valuable reference for future research on urea synthesis.