Magnetic Graphene Oxide-Supported Pd(0): A Novel Heterogeneous Nanocatalyst for Upgrading Sustainable Aminocarbonylation of Aryl and Heteroaryl Iodides
摘要
A novel heterogenous recoverable Fe₃O₄@GO–Melamine/TCT–Pd(0) nanocatalyst was successfully synthesized and applied as an efficient heterogeneous catalyst for palladium-catalyzed aminocarbonylation reactions. The catalyst was constructed through the immobilization of Pd(0) nanoparticles onto a nitrogen-rich melamine/triazine-functionalized graphene oxide support decorated with Fe₃O₄ magnetic nanoparticles. The prepared nanocomposite combined the high surface area and excellent stability of graphene oxide with the magnetic recoverability of Fe₃O₄ and the strong metal-coordinating ability of the melamine/TCT ligand framework. Comprehensive characterization of the catalyst was performed using FT-IR, XRD, BET, SEM, TEM, EDX, ICP-OES, XPS, TGA, and VSM analyses, confirming the successful formation of a stable and well-dispersed Pd(0)-based nanostructure. The catalytic activity of the synthesized material was investigated in aminocarbonylation reactions of various aryl iodides with different amines using Mo(CO)₆ as an in-situ carbon monoxide source. The reactions were efficiently carried out in a green PEG/H₂O solvent system under mild conditions, affording a wide range of amide derivatives in excellent yields (86–99%) within short reaction times. The catalyst demonstrated broad substrate compatibility, high catalytic efficiency, and excellent functional-group tolerance. Moreover, the magnetic nanocatalyst could be easily recovered using an external magnet and reused for up to nine consecutive cycles with minimal loss of catalytic activity, highlighting its excellent stability, recyclability, and potential applicability in sustainable organic synthesis.
Graphical Abstract