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A new class of actinide complexes [(L)An(N{SiMe 3 } 2 ) 3 ] (An = Th or U) ( Th1 - Th3 and U1-U3 ) supported by highly nucleophilic seven-membered N-heterocyclic iminato ligands were synthesized and fully characterized by single-crystal X-ray diffraction. These complexes were successfully exploited as powerful catalysts for the addition of alcohols to carbodiimides to yield the corresponding desirable isourea products at room temperature with short reaction times and excellent yields. Thorough stoichiometric, thermodynamic, and kinetic studies were carried out, allowing us to propose a plausible mechanism for the catalytic reaction.

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Remodeling of N-Heterocyclic Iminato Ligand Frameworks for the Facile Synthesis of Isoureas from Alcohols and Carbodiimides Promoted by Organoactinide (Th, U) Complexes