Environmentally Responsive Threading, Dethreading, and Fixation of Anion-Induced Pseudorotaxanes
Environmentally Responsive Threading, Dethreading, and Fixation of Anion-Induced Pseudorotaxanes
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DOI：
10.1021/ja109102k
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发表时间：
2011-02-09
影响因子：
15
通讯作者：
Sessler, Jonathan L.
中科院分区：
文献类型：
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作者：
Gong, Han-Yuan;Rambo, Brett M.;Sessler, Jonathan L.
四阳离子大环cyclo[2](2，6-di(1H-imidazol-1-yl)pridine)[2](1，4-dimethylenebenzene)六氟磷酸盐(1(4+).4PF(6)(-))作为一个大的、灵活的“分子盒”，支持环境响应阴离子诱导的假轮烷的形成，以及其他扩展结构，包括金属连接的超分子多轮烷。具体地说，由4，4‘-联苯二羧酸和2，6-萘二甲酸衍生的四(4+)和双羧酸盐客体的结合导致了对环境刺激(包括pH和温度)变化的反应的假紫杉烷的形成。通过添加银(I)形式的金属连接物，可以将所得到的结构“锁定在适当的位置”；这产生了有序的金属连接的聚轮烷。用一维和二维(H-1和NOESY)核磁共振波谱、质谱仪(ESI-MS)和单晶X-射线衍射法对互穿结构进行了表征。
The tetracationic macrocycle cyclo[2](2,6-di(1H-imidazol-1-yl)pridine)[2](1,4-dimethylenebenzene) hexafluorophosphate (1(4+) .4PF(6)(-)) acts as a large, flexible "molecular box" that supports the formation of environmentally responsive anion-induced pseudorotaxanes, as well as other extended structures, including metal-linked supramolecular polyrotaxanes. Specifically, the combination of the tetracation 1(4+) and bis-carboxylate guests derived from 4,4'-biphenyldicarboxylic acid and 2,6-naphthalenedicarboxylic acid results in the formation of pseudorotaxanes that respond to changes in environmental stimuli, including pH and temperature. The resulting structures can be "locked into place" via the addition of a metal-linker in the form of Ag(I); this gives rise to an ordered metal-linked polyrotaxane. The interpenetrated constructs described in this article were characterized in solution and in the solid state by one- and two-dimensional (H-1 and NOESY) NMR spectroscopy, as well as by mass spectrometry (ESI-MS) and single-crystal X-ray diffraction methods.