Artículo
Ruthenium(II) Complexes Containing Lutidine-derived Pincer CNC Ligands: Synthesis, Structure and Catalytic Hydrogenation of C=N bonds
Autor/es | Hernández Juárez, Martín
López Serrano, Joaquín Lara Muñoz, Patricia Morales Cerón, Judith Vaquero Gutiérrez, Mónica Álvarez González, Eleuterio Salazar Pereda, Verónica Suárez Escobar, Andrés Luis |
Fecha de publicación | 2015 |
Fecha de depósito | 2018-08-10 |
Publicado en |
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Resumen | A series of Ru complexes containing lutidine‐derived pincer CNC ligands have been prepared by transmetalation with the corresponding silver‐carbene derivatives. Characterization of these derivatives shows both mer and fac ... A series of Ru complexes containing lutidine‐derived pincer CNC ligands have been prepared by transmetalation with the corresponding silver‐carbene derivatives. Characterization of these derivatives shows both mer and fac coordination of the CNC ligands depending on the wingtips of the N‐heterocyclic carbene fragments. In the presence of tBuOK, the Ru‐CNC complexes are active in the hydrogenation of a series of imines. In addition, these complexes catalyze the reversible hydrogenation of phenantridine. Detailed NMR spectroscopic studies have shown the capability of the CNC ligand to be deprotonated and get involved in ligand‐assisted activation of dihydrogen. More interestingly, upon deprotonation, the Ru‐CNC complex 5 e(BF4) is able to add aldimines to the metal–ligand framework to yield an amido complex. Finally, investigation of the mechanism of the hydrogenation of imines has been carried out by means of DFT calculations. The calculated mechanism involves outer‐sphere stepwise hydrogen transfer to the CN bond assisted either by the pincer ligand or a second coordinated H2 molecule. |
Agencias financiadoras | Ministerio de Ciencia e Innovación (MICIN). España Junta de Andalucía |
Cita | Hernández Juárez, M., López Serrano, J., Lara Muñoz, P., Morales Cerón, J., Vaquero Gutiérrez, M., Álvarez González, E.,...,Suárez Escobar, A.L. (2015). Ruthenium(II) Complexes Containing Lutidine-derived Pincer CNC Ligands: Synthesis, Structure and Catalytic Hydrogenation of C=N bonds. Chemistry - a European Journal, 21 (20), 7540-7555. https://10.1002/chem.201406040. |
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