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• W1977308332 endingPage "6183" @default.
• W1977308332 startingPage "6172" @default.
• W1977308332 abstract "The triiron clusters Fe3(CO)9(μ3-EMLn)2 (1-E, MLn = MnCp(CO)2, E = P, As, Sb; 2-E, MLn = Cr(CO)5, E = P, As, Sb) can be considered cluster analogues of organopnictane (ER3) ligands, in which the triply bridging E ligands are coordinated to 16-electron capping metal groups, MLn. Structural parameters, infrared CO stretching frequencies, and reduction potentials for this metallopnictane series are reported. Analysis of structural, spectroscopic, and electrochemical data reveal systematic variations as a function of the capping heteroatom and the metal fragment coordinated to the heteroatom. The covalent radius of the capping heteroatom dictates the structure of the Fe3(CO)9(μ3-E)2 bonding framework, and both Fe−E and Fe−Fe distances increase linearly with increasing heteroatom covalent radius. The electronegativity of the capping heteroatom (E) influences the frequencies of the Fe3-core carbonyl stretching modes (νCO(Sb) < νCO(As) < νCO(P)), while the two-electron reduction potentials for the series 1 and series 2 clusters (E1/2(Sb) > E1/2(As) > E1/2(P)) correlate with the covalent radius of E. Clusters with capping Cr(CO)5 groups are reduced at potentials ∼400 mV more positive than the MnCp(CO)2-capped analogues. On the basis of the frequencies of the CO stretching modes for the capping MLn group and the E−MLn distance, the metallopnictance ligands are classified as intermediate between organopnictanes and halopnictanes in terms of their net electronic impact (the sum of σ-donating and π-accepting properties). Results of Fenske−Hall molecular orbital calculations provide a qualitative description of the Fe3−E2 bonding as a function of heteroatom (E). Trends in Mulliken populations and a Walsh analysis suggest the Fe−E bonds are strongest for the most electronegative E, phosphorus. The Fe−Fe overlap populations are nearly constant with E, despite the increase in Fe−Fe distance attendant upon incorporation of larger heteroatoms. Two-electron reduction of the metallopnictane Fe3-core changes the donor and acceptor characteristics of the metallopnictane ligand, as demonstrated by a structure determination for [(PhCH2)Me3N]2(1-P). The Mn−P distance in (1-P)2- is 0.1 Å longer than in the neutral analogue, 1-P. Single-crystal X-ray structure determinations for 1-As, 1-Sb, 2-P, 2-As, 2-Sb, and [(PhCH2)Me3N]2(1-P) are reported." @default.
• W1977308332 created "2016-06-24" @default.
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• W1977308332 date "1997-12-01" @default.
• W1977308332 modified "2023-10-11" @default.
• W1977308332 title "Structures, Bonding, Infrared Spectroscopy, and Two-Electron Reduction Potentials of the Coordinated Metallopnictanes Fe₃(CO)₉(μ₃-EML<i>_n</i>)₂ (E = P, As, Sb; ML<i>_n</i> = Cr(CO)₅, MnCp(CO)₂)" @default.
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• W1977308332 doi "https://doi.org/10.1021/ic970786a" @default.
• W1977308332 hasPublicationYear "1997" @default.
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