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• W2013354669 endingPage "6272" @default.
• W2013354669 startingPage "6257" @default.
• W2013354669 abstract "The iron complexes CpFe(PPh2NBn2)Cl (1-Cl), CpFe(PPh2NPh2)Cl (2-Cl), and CpFe(PPh2C5)Cl (3-Cl)(where PPh2NBn2 is 1,5-dibenzyl-1,5-diaza-3,7-diphenyl-3,7-diphosphacyclooctane, PPh2NPh2 is 1,3,5,7-tetraphenyl-1,5-diaza-3,7-diphosphacyclooctane, and PPh2C5 is 1,4-diphenyl-1,4-diphosphacycloheptane) have been synthesized and characterized by NMR spectroscopy, electrochemical studies, and X-ray diffraction. These chloride derivatives are readily converted to the corresponding hydride complexes [CpFe(PPh2NBn2)H (1-H), CpFe(PPh2NPh2)H (2-H), CpFe(PPh2C5)H (3-H)] and H2 complexes [CpFe(PPh2NBn2)(H2)]BArF4, [1-H2]BArF4, (where BArF4 is B[(3,5-(CF3)2C6H3)4]−), [CpFe(PPh2NPh2)(H2)]BArF4, [2-H2]BArF4, and [CpFe(PPh2C5)(H2)]BArF4, [3-H2]BArF4, as well as [CpFe(PPh2NBn2)(CO)]BArF4, [1-CO]Cl. Structural studies are reported for [1-H2]BArF4, 1-H, 2-H, and [1-CO]Cl. The conformations adopted by the chelate rings of the PPh2NBn2 ligand in the different complexes are determined by attractive or repulsive interactions between the sixth ligand of these pseudo-octahedral complexes and the pendant N atom of the ring adjacent to the sixth ligand. An example of an attractive interaction is the observation that the distance between the N atom of the pendant amine and the C atom of the coordinated CO ligand for [1-CO]BArF4 is 2.848 Å, considerably shorter than the sum of the van der Waals radii of N and C atoms. Studies of H/D exchange by the complexes [1-H2]+, [2-H2]+, and [3-H2]+ carried out using H2 and D2 indicate that the relatively rapid H/D exchange observed for [1-H2]+ and [2-H2]+ compared to [3-H2]+ is consistent with intramolecular heterolytic cleavage of H2 mediated by the pendant amine. Computational studies indicate a low barrier for heterolytic cleavage of H2. These mononuclear FeII dihydrogen complexes containing pendant amines in the ligands mimic crucial features of the distal Fe site of the active site of the [FeFe]-hydrogenase required for H–H bond formation and cleavage." @default.
• W2013354669 created "2016-06-24" @default.
• W2013354669 creator A5018967285 @default.
• W2013354669 creator A5022980951 @default.
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• W2013354669 creator A5063649936 @default.
• W2013354669 creator A5082146943 @default.
• W2013354669 creator A5090105637 @default.
• W2013354669 date "2012-03-29" @default.
• W2013354669 modified "2023-10-02" @default.
• W2013354669 title "Synthesis, Characterization, and Reactivity of Fe Complexes Containing Cyclic Diazadiphosphine Ligands: The Role of the Pendant Base in Heterolytic Cleavage of H₂" @default.
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