Department of Chemistry, University of Cambridge, Lensfield Road, Cambridge CB21EW, UK.
Org Biomol Chem. 2018 Jun 6;16(22):4183-4190. doi: 10.1039/c8ob00819a.
Synthetic oligomers equipped with complementary H-bond donor and acceptor side chains form multiply H-bonded duplexes in organic solvents. Comparison of the duplex forming properties of four families of oligomers with different backbones shows that formation of an extended duplex with three or four inter-strand H-bonds is more challenging than formation of complexes that make only two H-bonds. The stabilities of 1 : 1 complexes formed between length complementary homo-oligomers equipped with either phosphine oxide or phenol recognition modules were measured in toluene. When the backbone is very flexible (pentane-1,5-diyl thioether), the stability increases uniformly by an order of magnitude for each additional base-pair added to the duplex: the effective molarities for formation of the first intramolecular H-bond (duplex initiation) and subsequent intramolecular H-bonds (duplex propagation) are similar. This flexible system is compared with three more rigid backbones that are isomeric combinations of an aromatic ring and methylene groups. One of the rigid systems behaves in exactly the same way as the flexible backbone, but the other two do not. For these systems, the effective molarity for formation of the first intramolecular H-bond is the same as that found for the other two backbones, but additional H-bonds are not formed between the longer oligomers. The effective molarities are too low for duplex propagation in these systems, because the oligomer backbones cannot adopt conformations compatible with formation of an extended duplex.
合成的寡聚物配备互补的氢键供体和受体侧链,在有机溶剂中形成多重氢键双链。比较具有不同骨架的四组寡聚物的双链形成性质表明,形成具有三个或四个链间氢键的扩展双链比形成仅形成两个氢键的复合物更具挑战性。在甲苯中测量了配备膦氧化物或苯酚识别模块的长度互补同寡聚物之间形成的 1:1 复合物的稳定性。当骨架非常灵活(戊烷-1,5-二基硫醚)时,每个双链添加一个额外碱基对都会使稳定性均匀增加一个数量级:形成第一个分子内氢键(双链起始)和随后的分子内氢键(双链传播)的有效摩尔浓度相似。将该柔性体系与三个刚性骨架进行比较,刚性骨架是芳环和亚甲基的异构体组合。其中一个刚性系统的行为与柔性骨架完全相同,但另外两个则不然。对于这些系统,形成第一个分子内氢键的有效摩尔浓度与其他两个骨架相同,但较长的寡聚物之间没有形成额外的氢键。由于寡聚物骨架不能采用与扩展双链形成兼容的构象,因此这些系统中的双链传播的有效摩尔浓度太低。