Hydrogen transfer reaction to imines with 2-propanol catalyzed by ruthenium (II) complexes containing nitrogen-phosphorus (NPN) ligands. Experimental and computational studies

Camila Negrete-Vergara, Andrés Vega, Plinio Cantero-López, Osvaldo Yáñez, Sergio A. Moya, Gonzalo Valdebenito, Sebastián Parra-Melipan, Pedro Aguirre

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Resumen

This work reports the synthesis and characterization of ruthenium(II) complexes containing nitrogen-phosphorus-nitrogen (NPN) ligands, with L1 = N-(phenyl(pyridin-2-ylamino)phosphino)pyridin-2-amine and L2 = 4-methyl-N-((4-methylpyridin-2-ylamino)(phenyl)phosphino)pyridin-2-amine. The ruthenium complexes RuCl2PPh3(L1) (1) and RuCl2PPh3(L2) (2) show high activities in catalytic transfer hydrogenation of different substituted benzylideneanilines, with turnover frequencies up to 5882 h−1 and 5294 h−1, respectively. The RuCl(CO)PPh3(L1) (3) and RuCl(CO)PPh3(L2) (4) complexes were non-active in the reaction studied. Theoretical calculations conducted for complex 4 showed that the carbonyl group promotes σ-orbital interactions and backdonation phenomena from the metal centre to the π* orbitals in the CO ligand, presenting a strong orbital contribution. This supports the hypothesis that complexes 3 and 4 are less reactive species and therefore present poor or null catalytic performance in the reaction studied.

Idioma originalInglés
Número de artículo122064
PublicaciónInorganica Chimica Acta
Volumen568
DOI
EstadoPublicada - 1 ago. 2024

Áreas temáticas de ASJC Scopus

  • Química física y teórica
  • Química inorgánica
  • Química de los materiales

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