Brady Kimberly G, Liu Bingqing, Li Xiaopeng, Isaacs Lyle
Department of Chemistry and Biochemistry, University of Maryland, College Park, Maryland 20742, United States.
Department of Chemistry, University of South Florida, Tampa, Florida 33620, United States.
Supramol Chem. 2021;33(1-2):8-32. doi: 10.1080/10610278.2021.1908546. Epub 2021 Jun 2.
We report preparation of (bis)aniline ligand which contains a central viologen binding domain and its subcomponent self-assembly with aldehyde and Fe(OTf) in CHCN to yield tetrahedral assembly . Complexation of ligand with CB[7] in the form of CB[7]••2PF allows the preparation of assembly which contains an average of 1.95 (range 1-3) mechanically interlocked CB[7] units. Assemblies and are hydrolytically unstable in water due to their imine linkages. Redesign of our system with water stable 2,2'-bipyridine end groups was realized in the form of ligands and which also contain a central viologen binding domain. Self-assembly of with Fe(NTf) gave tetrahedral MOP as evidenced by H NMR, DOSY, and mass spectrometric analysis. In contrast, isomeric ligand underwent self-assembly with Fe(OTf) to give cubic assembly . Precomplexation of ligands and with CB[7] gave the acetonitrile soluble CB[7]••2PF and CB[7]••2PF complexes. Self-assembly of CB[7]••2PF with Fe(OTf) gave tetrahedron which contains on average 1.8 mechanically interlocked CB[7] units as determined by H NMR, DOSY, and ESI-MS analysis. Self-assembly of CB[7]••2PF with Fe(OTf) gave cube which contains 6.59 mechanically interlocked CB[7] units as determined by H NMR and DOSY measurements.
我们报道了含中心紫精结合域的（双）苯胺配体的制备，以及其亚组分与醛和三氟甲磺酸铁（Fe(OTf)）在乙腈中自组装生成四面体组装体的过程。配体与葫芦[7]（CB[7]）以CB[7]••2PF的形式络合，可制备出平均含有1.95个（范围为1 - 3个）机械互锁CB[7]单元的组装体。组装体和由于其亚胺键在水中水解不稳定。我们以配体和的形式实现了具有水稳定的2,2'-联吡啶端基的体系重新设计，它们同样含有中心紫精结合域。配体与三氟甲磺酸铁（Fe(NTf)）自组装得到四面体金属有机多面体（MOP），这通过核磁共振氢谱（H NMR）、扩散排序谱（DOSY）和质谱分析得以证实。相比之下，异构体配体与三氟甲磺酸铁（Fe(OTf)）自组装得到立方组装体。配体和与CB[7]预络合得到可溶于乙腈的CB[7]••2PF和CB[7]••2PF络合物。CB[7]••2PF与三氟甲磺酸铁（Fe(OTf)）自组装得到四面体，通过核磁共振氢谱（H NMR）、扩散排序谱（DOSY）和电喷雾电离质谱（ESI-MS）分析确定其平均含有1.8个机械互锁的CB[7]单元。CB[7]••2PF与三氟甲磺酸铁（Fe(OTf)）自组装得到立方体，通过核磁共振氢谱（H NMR）和扩散排序谱（DOSY）测量确定其含有6.59个机械互锁的CB[7]单元。
