Hunter Christopher A, Tomas Salvador
Centre for Chemical Biology, Krebs Institute for Biomolecular Science, Department of Chemistry, University of Sheffield, Sheffield S3 7HF UK.
J Am Chem Soc. 2006 Jul 12;128(27):8975-9. doi: 10.1021/ja061928f.
Linear oligomeric supramolecular assemblies of defined length have been generated using the Vernier principle. Two molecules, containing a different number (n and m) of mutually complementary binding sites, separated by the same distance, interact with each other to form an assembly of length (n x m). The assembly grows in the same way as simple supramolecular polymers, but at a molecular stop signal, when the binding sites come into register, the assembly terminates giving an oligomer of defined length. This strategy has been realized using tin and zinc porphyrin oligomers as the molecular building blocks. In the presence of isonicotinic acid, a zinc porphyrin trimer and a tin porphyrin dimer form a 3:4 triple stranded Vernier assembly six porphyrins long. The triple strand Vernier architecture introduced here adds an additional level of cooperativity, yielding a stability and selectivity that cannot be achieved via a simple Vernier approach. The assembly properties of the system were characterized using fluorescence titrations and size-exclusion chromatography (SEC). Assembly of the Vernier complex is efficient at micromolar concentrations in nonpolar solvents, and under more competitive conditions, a variety of fragmentation assemblies can be detected, allowing determination of the stability constants for this system and detailed speciation profiles to be constructed.
利用游标原理生成了具有确定长度的线性寡聚超分子组装体。两个分子,含有不同数量(n和m)的相互互补的结合位点,且间隔相同距离,它们相互作用形成长度为(n×m)的组装体。该组装体的生长方式与简单的超分子聚合物相同,但在分子终止信号处,当结合位点对齐时,组装体终止,从而得到具有确定长度的寡聚物。已使用锡卟啉和锌卟啉寡聚物作为分子构建块实现了这一策略。在异烟酸存在下,锌卟啉三聚体和锡卟啉二聚体形成一个六卟啉长的3:4三链游标组装体。这里引入的三链游标结构增加了额外的协同作用水平,产生了通过简单游标方法无法实现的稳定性和选择性。使用荧光滴定和尺寸排阻色谱(SEC)对该系统的组装性质进行了表征。在非极性溶剂中,微摩尔浓度下游标复合物的组装效率很高,在更具竞争性的条件下,可以检测到各种片段组装体,从而可以确定该系统的稳定性常数并构建详细的物种分布图谱。