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• W1976673042 abstract "A family of Ru 2 (II,II) and Ru 2 (II,III) tetracarboxylate complexes containing the bulky ligand 2,4,6-triisopropylbenzoate have been used to investigate the effect of internal rotation on the metal–metal bond length and electronic properties. A series of Ru 2 II,III complexes containing the bulky carboxylate ligand 2,4,6-triisopropylbenzoate (TiPB) of type trans -[Ru 2 (TiPB) 2 (O 2 CCH 3 ) 2 X] [X = Cl ( 1 ), PF 6 ( 2 )] and [Ru 2 (TiPB) 4 X] [X = Cl ( 3 ), PF 6 ( 4 )] have been synthesised. The corresponding Ru 2 II,II complexes trans -[Ru 2 (TiPB) 2 (O 2 CCH 3 ) 2 ] ( 5 ) and [Ru 2 (TiPB) 4 ] ( 6 ) were also isolated. Magnetic susceptibility measurements indicate that the diruthenium cores have the expected three ( 1 – 4 ) or two ( 5 and 6 ) unpaired electrons consistent with σ 2 π 4 δ 2 (δ ∗ π ∗ ) 3 and σ 2 π 4 δ 2 δ ∗2 π ∗2 electronic configurations. Compounds 1 – 4 and 6 were structurally characterised by X-ray crystallography, and show the expected paddlewheel arrangement of carboxylate ligands around the diruthenium core. The diruthenium cores of complexes 3 , 4 and 6 are all distorted to minimise steric interactions between the bulky carboxylate ligands. The Ru–Ru bond length in the Ru 2 II,II complex 6 [2.2425(6) Å] is the shortest observed for a diruthenium tetracarboxylate and, surprisingly, is 0.014 Å shorter than in the analogous Ru 2 II,III complex 4 , despite an increase in the formal Ru–Ru bond order from 2.0 ( 6 ) to 2.5 ( 4 ). This is rationalised in terms of the extent of internal rotation, or distortion, about the diruthenium core. This was supported by density functional theory calculations on the model complexes [Ru 2 (O 2 CH) 4 ] and [Ru 2 (O 2 CH) 4 ] + , that demonstrate the relationship between Ru–Ru bond length and internal rotation. Electrochemical and electronic absorption data were recorded for all complexes in solution. Comparison of the data for the ‘ bis – bis ’ ( 1 , 2 and 5 ) and tetra-substituted ( 3 , 4 and 6 ) complexes indicates that the shortening of the Ru–Ru bond length results in a small increase in energy of the near-degenerate δ ∗ and π ∗ orbitals." @default.
• W1976673042 created "2016-06-24" @default.
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• W1976673042 date "2010-11-01" @default.
• W1976673042 modified "2023-09-26" @default.
• W1976673042 title "Unexpected structural and electronic effects of internal rotation in diruthenium paddlewheel complexes containing bulky carboxylate ligands" @default.
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• W1976673042 doi "https://doi.org/10.1016/j.ica.2010.07.024" @default.
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