期刊
ORGANOMETALLICS
卷 40, 期 2, 页码 231-241出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.organomet.0c00717
关键词
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资金
- Centre National de la Recherche Scientifique (CNRS)
- Universite Toulouse III, Paul Sabatier
- Institut Universitaire de France (IUF)
- Embassy of Yemen in Paris
- program Pause
The coordination chemistry of NHC core pincer-type PCP and PCN ligands with a Mn(I) center was studied, revealing that Mn(I) complexes with bidentate and tridentate ligands exhibit different catalytic activities based on ligand structure.
The coordination chemistry of NHC core pincer-type PCP and PCN ligands with a Mn(I) center was systematically investigated. The reaction of [Mn(CO)(5)Br] with free carbenes, conveniently prepared from the corresponding imidazolium salts and a strong base, leads to the initial formation of bidentate fac[MnBr(CO)(3) (kappa P-2,C,L)] complexes bearing a pending phosphine or pyridine donor extremity (L), which upon bromide abstraction, afford cationic [Mn(CO)(3)(kappa P-3,C,L)](OTf) derivatives exhibiting a meridional or a facial coordinating geometry of tridentate NHC core ligand depending on its relative flexibility. All bi- and tridentate Mn(I) complexes were characterized by X-ray diffraction analysis. The impact of the tridentate ligand structure on catalytic performance was illustrated in the Mn-catalyzed hydrogenation of acetophenone revealing fac-[Mn(CO)(3)(kappa P-3,C,N)](OTO based on a 5,6-membered metallacyclic architecture to be the most active, thus evidencing the role of the pyridine arm lability in the catalytic cycle.
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