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首页> 外文期刊>Chemistry: A European journal >Modulation of a Supramolecular Bowl and Pot by Changing Solvent Systems and/or Metal/Ligand Ratios
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Modulation of a Supramolecular Bowl and Pot by Changing Solvent Systems and/or Metal/Ligand Ratios

机译：通过更改溶剂系统和/或金属/配体比率来调制超分子碗和锅

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摘要

A resorcin[4]arene-based ligand 2a with four p9yrimidine substituents at the upper rim was synthesized, and the generation of different metal-mediated superstructures from the same ligand and metal ions utilizing the unfavorable incorporation of the third and fourth Pd~II ions to ligand 2a was investigated. The supramolecular bowl 3a, which comes from a 1:2 combination of ligand 2a and [Pd(en)(NO_3)_2], was obtained in water even though excess of Pd_II complexes were employed. By adding methanol, the supramolecular pot 4 gradually formed, which was the major product when the ratio of mixed solvent reached methanol/water =5:1 (v/v). Host-guest complexation phenomena of 3a toward several aromatic carboxylates were demonstrated by isothermal titration calorimetry (ITC) and by ~1H NMR spectroscopy; both the enthalpy gain from electrostatic and hydrophobic interactions, and the entropygain from desolvation cooperatively contribute to the binding of anionically charged guests. The crystal structure of supramolecular pot 4 shows direct evidence for the hydrogen bonding between water and the armatic pi electrons in the solid state. The modulation between supramolecular bowl 3a and pot 4 was also made possible by changing the metal/ligand ratios in aqueous methanol solution as well as by varying the water content of the mixed solvent.
机译：合成了在上边缘具有四个p9yrimidine取代基的间苯二酚[4]芳烃基配体2a，并且利用第三和第四Pd〜II离子的不利结合，由相同的配体和金属离子生成了不同的金属介导的超结构研究了对配体2a的结合。即使使用过量的Pd_II复合物，也可以在水中获得由配体2a和[Pd（en）（NO_3）_2]的1：2组合形成的超分子碗3a。通过添加甲醇，逐渐形成超分子罐4，当混合溶剂的比例达到甲醇/水= 5：1（v / v）时，它是主要产物。通过等温滴定热法（ITC）和〜1H NMR光谱证明了3a对几种芳香族羧酸盐的主客体络合现象。静电和疏水相互作用的焓增加以及去溶剂化的熵增益都共同促进了带阴离子的客人的结合。超分子锅4的晶体结构直接证明了固态时水与电枢π电子之间存在氢键。通过改变甲醇水溶液中的金属/配体比率以及通过改变混合溶剂的水含量，也使得超分子碗3a和锅4之间的调节成为可能。

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