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首页> 外文期刊>Organometallics >Tris(alkyne) and bis(alkyne) complexes of coinage metals: Synthesis and characterization of (cyclooctyne)3_M~+ (M = Cu, Ag) and (cyclooctyne)2_Au~+ and coinage metal (M = Cu, Ag, Au) family group trends
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Tris(alkyne) and bis(alkyne) complexes of coinage metals: Synthesis and characterization of (cyclooctyne)3_M~+ (M = Cu, Ag) and (cyclooctyne)2_Au~+ and coinage metal (M = Cu, Ag, Au) family group trends

机译：造币金属的三（炔）和双（炔）配合物:(环辛炔）3_M〜+（M = Cu，Ag）和（环辛炔）2_Au〜+与造币金属（M = Cu，Ag，Au）的合成与表征家庭组趋势

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摘要

The tris(alkyne) copper complex [(cyclooctyne)_3Cu][SbF_6] has been synthesized using cyclooctyne and in situ generated CuSbF_6. Tris(alkyne) silver complexes [(cyclooctyne)_3Ag]~+ involving weakly coordinating counterions such as [SbF_6]~- and [PF_6]~- have also been isolated in good yield using cyclooctyne and commercially available AgSbF_6 and AgPF_6. These coinage metal tris(alkyne) adducts have trigonal-planar metal sites. The alkyne carbon atoms and the metal site form distorted spoke-wheel (rather than upright trigonal-prismatic) structures in the solid state. In [(cyclooctyne)_3Cu][SbF_6], these distortions result in a propeller-like arrangement of alkynes. A cationic gold(I) complex having two alkynes has been prepared by a reaction of equimolar amounts of Au(cyclooctyne)_2Cl and AgSbF_6 in dichloromethane. The gold atom of [(cyclooctyne)_2Au]~+ coordinates to the cyclooctynes in a linear fashion, while the carbon atoms of the alkyne groups form a tetrahedron around gold(I). Optimized geometries of cationic [(cyclooctyne)_3M]~+, [(cyclooctyne)_2M]~+, and [(cyclooctyne)_M]~+ and neutral [(cyclooctyne)_2MCl] and [(cyclooctyne)_MCl] adducts (M = Cu, Ag, Au) using density functional theory (DFT) at the BP86/def2-TZVPP level of theory and a detailed analysis of metal-alkyne bonding interactions are also presented.
机译：使用环辛炔和原位生成的CuSbF_6合成了三（炔）铜络合物[（cyclooctyne）_3Cu] [SbF_6]。还使用环辛炔和可商购的AgSbF_6和AgPF_6以良好的产率分离了包括弱配位抗衡离子如[SbF_6]〜-和[PF_6]〜-的三（炔）银配合物[（环辛炔）_3Ag]〜+。这些造币金属三（炔）加合物具有三角平面的金属位点。炔烃碳原子和金属位点在固态时形成扭曲的辐条轮（而不是直立的三角棱柱形）结构。在[（cyclooctyne）_3Cu] [SbF_6]中，这些变形导致炔烃呈螺旋桨状排列。通过使等摩尔量的Au（环辛炔）_2Cl和AgSbF_6在二氯甲烷中反应，制备了具有两个炔烃的阳离子金（I）络合物。 [（环辛炔）_2Au] +的金原子以线性方式与环辛炔配位，而炔基的碳原子在金（I）周围形成四面体。阳离子[（cyclooctyne）_3M]〜+，[（cyclooctyne）_2M]〜+和[（cyclooctyne）_M]〜+和中性​​[[cyclooctyne）_2MCl]和[（cyclooctyne）_MCl]加合物的最佳几何构型（M =铜，银，金）在BP86 / def2-TZVPP的理论水平上使用密度泛函理论（DFT）进行了介绍，并对金属-炔键相互作用进行了详细分析。

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