C7 and C9 carbon-rich bridges in diruthenium systems: synthesis, spectroscopic, and theoretical investigations of different oxidation States

Journal of the American Chemical Society
Stéphane RigautDaniel Touchard

Abstract

Two methodologies of C-C bond formation to achieve organometallic complexes with 7 or 9 conjugated carbon atoms are described. A C7 annelated trans-[Cl(dppe)2Ru=C=C=C-CH=C(CH2)-C[triple bond]C-Ru(dppe)2Cl][X] (X = PF6, OTf) complex is obtained from the diyne trans-[Cl(dppe)2Ru-(C[triple bond]C)2-R] (R = H, SiMe3) in the presence of [FeCp2][PF6] or HOTf, and C7 or C9 complexes trans-[Cl(dppe)2Ru-(C[triple bond]C)n-C(CH3)=C(R1)-C(R2)=C=C=Ru(dppe)2Cl][X] (n = 1, 2; R1 = Me, Ph, R2 = H, Me; X = BF4, OTf) are formed in the presence of a polyyne trans-[Cl(dppe)2Ru-(C[triple bond]C)n-R] (n = 2, 3; R = H, SiMe3) with a ruthenium allenylidene trans-[Cl(dppe)2Ru=C=C=C(CH2R1)R2][X]. These reactions proceed under mild conditions and involve cumulenic intermediates [M+]=(C=)nCHR (n = 3, 5), including a hexapentaenylidene. A combination of chemical, electrochemical, spectroscopic (UV-vis, IR, NIR, EPR), and theoretical (DFT) techniques is used to show the influence of the nature and conformation of the bridge on the properties of the complexes and to give a picture of the electron delocalization in the reduced and oxidized states. These studies demonstrate that the C7 bridging ligand spanning the metal centers by almost 12 angstroms is impli...Continue Reading

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Citations

Sep 9, 2011·Accounts of Chemical Research·Cecilia ColettiNazzareno Re
Aug 3, 2013·Inorganic Chemistry·Daniel E HainesMichael D Hopkins
Jul 20, 2007·Chemical Communications : Chem Comm·Céline OlivierStéphane Rigaut
Dec 17, 2008·Chemical Communications : Chem Comm·Yifei LiuStéphane Rigaut
Dec 4, 2015·Dalton Transactions : an International Journal of Inorganic Chemistry·Jing ZhangSheng Hua Liu
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Apr 23, 2014·Chemistry : a European Journal·Samuel De SousaCéline Olivier
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Apr 19, 2007·Chemistry, an Asian Journal·Thomas C W Mak, Liang Zhao
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Nov 22, 2017·Inorganic Chemistry·Emmanuel Di PiazzaStéphane Rigaut
May 22, 2007·Inorganic Chemistry·Li-Bin GaoZhong-Ning Chen

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