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首页> 美国卫生研究院文献>Chemical Science >Synthesis structure and reactivity of a terminal magnesium fluoride compound TpButMeMgF: hydrogen bonding halogen bonding and C–F bond formation
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Synthesis structure and reactivity of a terminal magnesium fluoride compound TpButMeMgF: hydrogen bonding halogen bonding and C–F bond formation

机译：末端氟化镁化合物TpButMe MgF的合成结构和反应性：氢键卤素键和CF键的形成

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摘要

The bulky tris(3-tert-butyl-5-pyrazolyl)hydroborato ligand, [TpBut,Me], has been employed to obtain the first structurally characterized example of a molecular magnesium compound that features a terminal fluoride ligand, namely [TpBut,Me]MgF, via the reaction of [TpBut,Me]MgMe with Me3SnF. The chloride, bromide and iodide complexes, [TpBut,Me]MgX (X = Cl, Br, I), can also be obtained by an analogous method using Me3SnX. The molecular structures of the complete series of halide derivatives, [TpBut,Me]MgX (X = F, Cl, Br, I) have been determined by X-ray diffraction. In each case, the Mg–X bond lengths are shorter than the sum of the covalent radii, thereby indicating that there is a significant ionic component to the bonding, in agreement with density functional theory calculations. The fluoride ligand of [TpBut,Me]MgF undergoes halide exchange with Me3SiX (X = Cl, Br, I) to afford [TpBut,Me]MgX and Me3SiF. The other halide derivatives [TpBut,Me]MgX undergo similar exchange reactions, but the thermodynamic driving forces are much smaller than those involving fluoride transfer, a manifestation of the often discussed silaphilicity of fluorine. In accord with the highly polarized Mg–F bond, the fluoride ligand of [TpBut,Me]MgF is capable of serving as a hydrogen bond and halogen bond acceptor, such that it forms adducts with indole and C6F5I. [TpBut,Me]MgF also reacts with Ph3CCl to afford Ph3CF, thereby demonstrating that [TpBut,Me]MgF may be used to form C–F bonds.
机译：庞大的三（3-叔丁基-5-吡唑基）氢硼酸盐配体[Tp Bu t ，Me ]已用于获得第一个结构特征的[Tp Bu t ，Me ] MegfF通过[Tp Bu t < / sup>，我]带有Me3SnF的MgMe。氯化物，溴化物和碘化物络合物[Tp Bu t ，Me ] MgX（X = Cl，Br，I），也可以通过类似的方法使用Me3SnX获得。卤化物衍生物[Tp Bu t ，Me ] MgX（X = F，Cl，Br，I）的完整系列的分子结构已通过X-确定射线衍射。在每种情况下，Mg-X键的长度都短于共价半径的总和，从而表明与键合功能理论计算相符，键中存在重要的离子成分。 [Tp Bu t ，Me ] MgF的氟化物配体与Me3SiX（X = Cl，Br，I）进行卤化物交换，得到[Tp Bu > t ，Me ] MgX和Me3SiF。其他卤化物衍生物[Tp Bu t ，Me ] MgX经历相似的交换反应，但热力学驱动力比涉及氟化物转移的热动力小得多，讨论了氟的硅亲合性。根据高极化的Mg-F键，[Tp Bu t ，Me ] MgF的氟化物配体可以用作氢键和卤素键受体，使其与吲哚和C6F5I形成加合物。 [Tp Bu t ，Me ] MgF也与Ph3CCl反应生成Ph3CF，从而证明[Tp Bu t ，Me < / sup>] MgF可用于形成CF键。

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