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• W2103299092 abstract "The reaction of [CpRu(iPr-DAB)(OTf)] (iPr-DAB = N,N′-diisopropyl-1,4-diaza-1,3-butadiene) with excess fumaronitrile yields [CpRu(iPr-DAB)(σN-fumaronitrile)][OTf] (1), which is in equilibrium with the binuclear complex [{CpRu(iPr-DAB)}2(μ-fumaronitrile)][OTf]2 (2) and free fumaronitrile. Complex 2 could be prepared quantitatively by the reaction of [CpRu(iPr-DAB)][OTf] with 0.5 equiv. of fumaronitrile. The reaction of [CpRu(PPh3)2][OTf] with excess fumaronitrile led to the monomeric complex [CpRu(PPh3)2(σN-fumaronitrile)][OTf] (3), while reaction with 0.5 equiv. of fumaronitrile gave [{CpRu(PPh3)2)2(μ-fumaronitrile)][OTf]2 (4) in 100% yield. Attempts to isolate the asymmetric compound [CpRu(iPr-DAB)(μ-fumaronitrile)CpRu(PPh3)2][OTf]2 (5) failed since in all cases a mixture of 2, 4 and the desired complex of 5 was formed. The redox behavior of complexes 1 and 2 was investigated by cyclic voltammetry and UV-Vis/IR spectroelectrochemistry. The chemically irreversible one-electron reduction of both complexes is localized on the fumaronitrile ligand, as was also found for the PPh3-substituted complexes 3 and 4. These results are in sharp contrast with the chemically reversible, iPr-DAB-localized one-electron reduction of the mononuclear derivatives [CpRu(iPr-DAB)(X)]+ (X = CO, PPh3). Oxidation of the RuII centers in 1 and 2 resulted in secondary chemical reactions. The final oxidation product in the case of the binuclear complex 2 has been unambiguously identified as the cation [CpRu(iPr-DAB)(OTf)]+. This result demonstrates that the RuIII-(σN-fumaronitrile) bond in the studied complexes is rather weak and easily dissociates. The oxidation-induced reactivity of 2 hence rules out the spectroscopic characterization of the mixed-valence RuIIRuIII intermediate 2+." @default.
• W2103299092 created "2016-06-24" @default.
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• W2103299092 date "1997-01-01" @default.
• W2103299092 modified "2023-09-24" @default.
• W2103299092 title "Synthesis and redox properties of [{CpRu(L2)}2-(μ-fumaronitrile)][OTf]2 and [CpRu(L2)(σN-fumaronitrile)][OTf] with L2 = N,N′-diisopropyl-1,4-diaza-1,3-butadiene (iPr-DAB) or L = PPh3" @default.
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• W2103299092 doi "https://doi.org/10.1016/s0020-1693(96)05161-4" @default.
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