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Synthesis, characterization, and reactivity of a high-spin iron(II) hydrido complex supported by a PNP pincer ligand and its application as a homogenous catalyst for the hydrogenation of alkenes

This study focused on the synthesis and characterization of a range of low-valent, high-spin iron(II) complexes supported by a carbazole-based PNP pincer-type ligand. The addition of the lithiated ligand (PNP)Li to FeCl2(THF)1.5 yielded the chlorido complex (PNP)FeCl (1), which could be readily conv...

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Bibliographische Detailangaben
Hauptverfasser: Ott, Jonas C. (Verfasst von) , Blasius, Clemens K. (Verfasst von) , Wadepohl, Hubert (Verfasst von) , Gade, Lutz H. (Verfasst von)
Dokumenttyp: Article (Journal)
Sprache:Englisch
Veröffentlicht: February 23, 2018
In: Inorganic chemistry
Year: 2018, Jahrgang: 57, Heft: 6, Pages: 3183-3191
ISSN:1520-510X
DOI:10.1021/acs.inorgchem.7b03227
Online-Zugang:Verlag, lizenzpflichtig, Volltext: https://doi.org/10.1021/acs.inorgchem.7b03227
Volltext
Verfasserangaben:Jonas C. Ott, Clemens K. Blasius, Hubert Wadepohl, Lutz. H. Gade
Beschreibung
Zusammenfassung:This study focused on the synthesis and characterization of a range of low-valent, high-spin iron(II) complexes supported by a carbazole-based PNP pincer-type ligand. The addition of the lithiated ligand (PNP)Li to FeCl2(THF)1.5 yielded the chlorido complex (PNP)FeCl (1), which could be readily converted to the four-coordinate iron(II) alkyl complexes (PNP)FeR [R = CH2SiMe3 (3a), Me (3b), CH2Ph (3c)]. These iron(II) complexes were fully characterized by X-ray analysis and a comprehensive, density-functional-theory-assisted study with complete assignment of their paramagnetic 1H and 13C NMR spectra. Treatment of 1 with KHBEt3 or the addition of molecular hydrogen to (PNP)FeR afforded a high-spin iron(II) PNP hydrido complex, which was identified as the dimer [(PNP)Fe(μ-H)]2 (4) with two bridging hydrido ligands between the iron centers. Exposing complexes 1 and 4 to carbon monoxide led to the corresponding six-coordinate, diamagnetic complexes (PNP)Fe(CO)2Cl (2) and (PNP)Fe(CO)2H (5), of which 2 was present as cis/trans isomers. Furthermore, 4 was found to be an active catalyst for the hydrogenation of alkenes.
Beschreibung:Gesehen am 12.03.2020
Beschreibung:Online Resource
ISSN:1520-510X
DOI:10.1021/acs.inorgchem.7b03227

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