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首页> 外文期刊>Chemistry: A European journal >Self-Assembled Organometallic [12]Metallacrown-3 Complexes
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Self-Assembled Organometallic [12]Metallacrown-3 Complexes

机译：自组装有机金属[12] Metallacrown-3配合物

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The reaction of [(arene)-RuCl_2]_2(arene=C_6H_6,cymene,C_6H_3Et_3,or C_6Me_6) or [CpRhCl_2]_2 with 3-hy-droxy-2-pyridone in the presence of Cs_2CO_3 gives trinuclear metallamacro-cyclic complexes .The self-assembly process was shown to be completely diastereoselective,and a racemic mix-ture of complexes with M_RM_RM_R or M_sM_sM_s(M=Ru,Rh)configuration was obtained.plausible mononuclear intermediates of the formula[(arene)-RuCl(C_5H_4NO_2)] (arene=cymene,C_6Me_6)have been isolated and charac-terized.A structurally related trimer was synthesized by using [(cymene)-RuCl_2]_2 and 3-acetamido-2-pyridone in -stead of 3-hydroxy-2-pyridone.The macrocyclec were shown to be highly potent ionphores for Na~+ and /or Li~+ with negligible affinities for the larger cation K~+ The selectivities of the re-ceptors depend on the #pi#-ligand present:whereas the (C_6H_6)Ru-and (cymene)-Ru complexes bind both Li~+and Na~+,the(C_6Me_6)Ru-,(C_6H_3E_3t)Ru-,and CpRh complexes bind exclusively Li~+.For all receptors,the presence of alkali metal ions can be detected electrochem-ically:the peak potential is shifted by>300mV toward anionic potential upon binding.This behavior was utilized to detect Li~+ and colorimetrically.Single crystal X-ray analyses have been carried out on eight complexes,four of which are bound to an alkali metal halide ion pair Structural parameters,which affect the affinity and selectivity are discussed .A computational study on [{MX}[12]crown-3]complexes(M=Li,Na;X=Cl,Br I)was performed in order to compare relevant bond lengths and angles of the energy-minimized structures with those of the organome-tallic receptors.
机译：[（芳烃）-RuCl_2] _2（芳烃= C_6H_6，cymene，C_6H_3Et_3，或C_6Me_6）或[CpRhCl_2] _2在Cs_2CO_3存在下与3-羟基-吡喃-2-吡啶酮反应得到三核金属环杂配合物。结果表明自组装过程是完全非对映选择性的，并获得了具有M_RM_RM_R或M_sM_sM_s（M = Ru，Rh）构型的配合物的外消旋混合物。式[[芳烃）-RuCl（C_5H_4NO_2）分离并表征了[芳烃= cymene，C_6Me_6]。用[（cymene）-RuCl_2] _2和3-乙酰氨基-2-吡啶酮代替3-羟基-2-合成了结构相关的三聚体。大环化合物被证明是Na〜+和/或Li〜+的高效离子电泳，对较大阳离子K〜+的亲和力可忽略不计。受体的选择性取决于存在的＃pi＃配体： （C_6H_6）Ru-和（cymene）-Ru配合物都结合Li〜+和Na〜+，（C_6Me_6）Ru-，（C_6H_3E_3t）Ru-和CpRh配合物仅结合Li〜+。可以电化学检测碱金属离子的存在：结合后峰电位向阴离子电位移动> 300mV。此行为用于检测Li〜+和比色法。进行了单晶X射线分析讨论了八个配合物，其中四个与碱金属卤化物离子对结合。讨论了影响亲和性和选择性的结构参数。[{MX} [12] crown-3]配合物（M = Li，为了比较能量最小化结构的相关键长和角度与有机金属受体的键长和角度，进行了Na; X = Cl，Br I）的反应。

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