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首页> 外文期刊>Chemistry: A European journal >Dynamic Equilibrium between a Supramolecular Capsule and Bowl Generated by Inter-and Intramolecular Metal Clipping
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Dynamic Equilibrium between a Supramolecular Capsule and Bowl Generated by Inter-and Intramolecular Metal Clipping

机译：分子间和分子内金属截留产生超分子胶囊和碗之间的动态平衡

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摘要

The metal-induced self-assembly of a resorcin[4]arene derivative 1 that has four pyridine units as pendent groups and two equivalents of[M(dppp)(OTf)_2](M = Pd,Pt)results in a dynamic equilibrium between an interclipped supramolecular capsule 3 and an intraclipped bowl 4 in nitrome-thane,although the interclipped capsule 3 is formed as a sole adduct in chloroform/methanol and the intraclipped bowl 4 is formed exclusively in an aqueous phase.This demonstrates how metal-induced self-assembly can be tuned by subtle changes in the solvent system.The coexistence of the two structures in nitromethane was characterized by NMR spectroscopy and coldspray ionization mass spectrometry(CSI-MS).The crystal structure of the interclipped capsule 3b,which is composed of two units of ligand 1 and four Pt11 ions,reveals the capsule cavity to have nanoscale dimensions of 15 x 20 A.NMR spectra show that the dynamic equilibrium between 3 and 4 is dependent on concentration and temperature.Temperature-dependent :H NMR spectroscopy was carried out from 273 to 343 K to verify the thermo-dynamic parameters that control the dynamic equilibrium process;the con version from the interclipped supra-molecular capsule 3 a to the intraclip ped bowl 4 a is entropically favored and enthalpically disfavored.The rota tional barrier of the restricted rotation of pyridine units in the intraclipped bowl 4 was determined by line-shape analysis.
机译：具有四个悬垂基团和两个当量[M（dppp）（OTf）_2]（M = Pd，Pt）的间苯二酚[4]芳烃衍生物1的金属诱导自组装导致动态平衡尽管夹层胶囊3是在氯仿/甲醇中形成的唯一加合物，而夹层碗4仅在水相中形成，但是夹层胶囊3在硝烟烷中的夹层超分子胶囊3和夹层碗4之间存在。可以通过溶剂系统的细微变化来调节自组装。通过NMR光谱和冷喷雾电离质谱（CSI-MS）表征硝基甲烷中两种结构的共存。夹层胶囊3b的晶体结构由由两个单位的配体1和四个Pt11离子组成，揭示了胶囊腔的纳米尺度尺寸为15 x 20 A.NMR谱图显示3和4之间的动态平衡取决于浓度和温度。 dent：H NMR光谱在273至343 K范围内进行，以验证控制动态平衡过程的热力学参数;从夹层超分子胶囊3a到夹带内腔的碗4a的转化有利于熵，通过线形分析确定内夹钳碗4中吡啶单元的受限旋转的旋转屏障。

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