Catalytic activity of a new Ru(ii) complex for the hydrogen transfer reaction of acetophenone and: N -benzylideneaniline: Synthesis, characterization and relativistic DFT approaches

C. Pérez-Zúñiga, C. Negrete-Vergara, Mauricio Yáñez, Pedro Aguirre, Ramiro Arratia-Pérez, César A. Zúñiga, Sergio A. Moya, PLINIO CANTERO LOPEZ

Research output: Contribution to journalArticle

Abstract

The synthesis and characterization of a new ruthenium(ii) complex containing a hemilabile P^N-ligand are reported. The catalytic activity of this complex was evaluated in the hydrogen transfer reaction of acetophenone and N-benzylideneaniline achieving conversions around 35 and 96% respectively. Condensed Fukui functions in a relativistic DFT scheme show that the regions for the electrophilic (f-) and nucleophilic (f+) attack are Cl- in the axial position, regions belonging to the P^N ligand and the metal center. The lability of the ligands is determined using different theoretical approaches like Morokuma-Ziegler energy decomposition analysis combined with the Extended Transition State with Natural Orbitals of Chemical Valence (ETS-NOCV). The major lability for the -Cl ligand (protic environment) is ideal for designing a new ruthenium hydride complex, suitable for catalytic applications. The σ-donation determines the degree of covalence of the chemical bond involving a lower trend to dissociate, as is the case of the P^N-ligand. The most important excitation energies appear in the region between 250 and 410 nm and are assigned to ligand to ligand charge transfer (LLCT) and metal to ligand charge transfer (MLCT) transitions.

Original languageEnglish
Pages (from-to)10545-10553
Number of pages9
JournalNew Journal of Chemistry
Volume43
Issue number26
DOIs
Publication statusPublished - 1 Jan 2019

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Discrete Fourier transforms
Hydrogen
Catalyst activity
Ligands
Ruthenium
Charge transfer
Metals
acetophenone
Excitation energy
Chemical bonds
Hydrides
Decomposition

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)
  • Materials Chemistry

Cite this

Pérez-Zúñiga, C. ; Negrete-Vergara, C. ; Yáñez, Mauricio ; Aguirre, Pedro ; Arratia-Pérez, Ramiro ; Zúñiga, César A. ; Moya, Sergio A. ; CANTERO LOPEZ, PLINIO. / Catalytic activity of a new Ru(ii) complex for the hydrogen transfer reaction of acetophenone and : N -benzylideneaniline: Synthesis, characterization and relativistic DFT approaches. In: New Journal of Chemistry. 2019 ; Vol. 43, No. 26. pp. 10545-10553.
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Catalytic activity of a new Ru(ii) complex for the hydrogen transfer reaction of acetophenone and : N -benzylideneaniline: Synthesis, characterization and relativistic DFT approaches. / Pérez-Zúñiga, C.; Negrete-Vergara, C.; Yáñez, Mauricio; Aguirre, Pedro; Arratia-Pérez, Ramiro; Zúñiga, César A.; Moya, Sergio A.; CANTERO LOPEZ, PLINIO.

In: New Journal of Chemistry, Vol. 43, No. 26, 01.01.2019, p. 10545-10553.

Research output: Contribution to journalArticle

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AU - Arratia-Pérez, Ramiro

AU - Zúñiga, César A.

AU - Moya, Sergio A.

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