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首页> 外文期刊>Chemistry: A European journal >Synthesis, Time-Resolved Luminescence, NMR Spectroscopy, Circular Dichroism and Circularly Polarised Luminescence Studies of Enantiopure Macrocyclic Lanthanide Tetraamide Complexes
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Synthesis, Time-Resolved Luminescence, NMR Spectroscopy, Circular Dichroism and Circularly Polarised Luminescence Studies of Enantiopure Macrocyclic Lanthanide Tetraamide Complexes

机译：对映纯大环镧系元素四酰胺配合物的合成，时间分辨发光，NMR光谱，圆二色性和圆偏振发光研究

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摘要

The syntheses and properties of a series of lanthanide complexes (Ln=Eu,Tb,Dy,Yb)of C_4 symmetric chiral tetraamide ligands based on 1,4,7,10-tetraazacyclododecane are reported. The configuration of the chiral centre at carbon in the amide substituent (CH_2NHCO-CH(Me)Ar) determines the helicity of the dervied complex and the configurationof the macrocyclic ring. The enantiopure lanthanide complexes do not undergo #DELTA#/#LAMBDA# interconversion in the termperature range 220 to 320 K and three complexes have been characterised by X-ray crystallography, revealing nine-coordination about the lanthanide ion (Ln=Eu,Dy)with a monocapped square-antiprismatic coordination geometry. The terbium complexes are highly emissive in aqueous solution following excitation into the aryl chromophore (e.g.for [Tb centre dot(R)-7a]~(3+) ~#phi#H_2O=0.49;#phi#D_2O=0.81) and all of the lanthanide complexes exhibit strong circularly polarised luminescence. The ytterbium complexes (e.g.[Yb centre dot (S)-5b]~(3+))shows a strong near-IR CD and circularly polarised luminescence (CPL) associated with the ~2F_(5/2)-~2F_(7/2) transition. Overall, these emissive complexes allow control in modulating both the frequency and the polarisation of emitted light in aqueous solution.
机译：报道了基于1,4,7,10-四氮杂十二烷的C_4对称手性四酰胺配体的一系列镧系元素配合物（Ln = Eu，Tb，Dy，Yb）的合成和性质。酰胺取代基（CH_2NHCO-CH（Me）Ar）中碳的手性中心构型决定了衍生复合物的螺旋度和大环的构型。对映体纯镧系元素在220至320 K的温度范围内不发生#DELTA＃/＃LAMBDA＃互变，并且X射线晶体学表征了三种配合物，揭示了镧系元素离子的9位配位（Ln = Eu，Dy）具有单峰方形反棱角坐标几何。激发进入芳基发色团后，aqueous络合物在水溶液中具有高发射率（例如[Tb center dot（R）-7a]〜（3+）〜＃phi＃H_2O = 0.49;＃phi＃D_2O = 0.81），所有镧系元素配合物表现出强的圆偏振发光。 complex配合物（例如[Yb中心点（S）-5b]〜（3+））显示出很强的近红外CD和与〜2F_（5/2）-〜2F_（7）相关的圆偏振发光（CPL） / 2）过渡。总的来说，这些发光络合物可以控制水溶液中发射光的频率和偏振。

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