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- W2321811454 endingPage "3258" @default.
- W2321811454 startingPage "3248" @default.
- W2321811454 abstract "Redox-active, highly symmetrical cubic octasilsesquioxanes (OS) peripherally decorated with 24 ferrocenyl units, linked in threes around the periphery of a cubic cage, namely, [Fc3Si(CH2)2Me2SiO]8Si8O12 (6) and [Fc3Si(CH2)2]8Si8O12 (7) (Fc = (η5-C5H4)Fe(η5-C5H5)), have been synthesized. Such integrally ferrocenyl-functionalized cubic macromolecules 6 and 7, as well as the related small-molecule models hexaferrocenyldisiloxane [Fc3Si(CH2)2Me2Si]2O (4) and dodecaferrocenyl cyclotetrasiloxane [Fc3Si(CH2)2MeSiO]4 (5), have been prepared by covalently linking, via Karstedt’s-catalyzed hydrosilylation, triferrocenylvinylsilane (CH2═CH)Si(Fc)3 (3) around the surface of octasilsesquioxane cages T8(OSiMe2H)8 and T8H8 and linear [Me2SiH]2O and cyclic [MeSiHO]4 siloxane scaffolds, respectively. All new polyferrocenyl oligosiloxanes have been thoroughly characterized using a combination of elemental analysis, multinuclear (1H, 13C, 29Si) NMR spectroscopy, FT-IR, and MALDI-TOF mass spectrometry. The molecular structure of disiloxane 4, in the solid state, has been determined by single-crystal X-ray analysis. Hexametallic 4 shows a bent arrangement of the ferrocenyl-substituted disiloxane linkage (Si–O–Si angle of 147.6(5)°). Polyferrocenyl-OS 6 and 7 show good thermal stability and form iron-containing ceramics when pyrolyzed under nitrogen. The electrochemical behavior of polyferrocenyl OS and model linear and cyclic siloxanes has been examined by cyclic and square wave voltammetries, in dichloromethane solution using PF6– and B(C6F5)4– as supporting electrolyte anions of different coordinating ability. The novel maximally ferrocenyl-functionalized oligosiloxanes exhibit a three-wave redox pattern, suggesting appreciable electronic interactions between the silicon-bridged triferrocenyl moieties as they are successively oxidized. OS 6 and 7 undergo remarkable oxidative precipitation in CH2Cl2/n-NBu4PF6 and are able to form stable electroactive films on platinum electrode surfaces. They are the first redox-active OS showing significant electronic interactions between metal sites on the cage surface." @default.
- W2321811454 created "2016-06-24" @default.
- W2321811454 creator A5011313760 @default.
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- W2321811454 creator A5065207297 @default.
- W2321811454 creator A5086637994 @default.
- W2321811454 creator A5089760806 @default.
- W2321811454 date "2012-03-19" @default.
- W2321811454 modified "2023-10-05" @default.
- W2321811454 title "Cubic Octasilsesquioxanes, Cyclotetrasiloxanes, and Disiloxanes Maximally Functionalized with Silicon-Bridged Interacting Triferrocenyl Units" @default.
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- W2321811454 doi "https://doi.org/10.1021/om300101w" @default.
- W2321811454 hasPublicationYear "2012" @default.
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