Itabashi Hiroki, Datta Sougata, Tsukuda Ryohei, Hollamby Martin J, Yagai Shiki
Division of Advanced Science and Engineering, Graduate School of Science and Engineering, Chiba University 1-33 Yayoi-cho, Inage-ku Chiba 263-8522 Japan.
Institute for Advanced Academic Research (IAAR), Chiba University 1-33 Yayoi-cho, Inage-ku Chiba 263-8522 Japan
Chem Sci. 2023 Mar 2;14(12):3270-3276. doi: 10.1039/d2sc07063d. eCollection 2023 Mar 22.
A judicious combination of ring-closing supramolecular polymerization and secondary nucleation can hierarchically organize a diphenylnaphthalene barbiturate monomer bearing a 3,4,5-tri(dodecyloxy)benzyloxy unit into self-assembled nano-polycatenanes composed of nanotoroids. In our previous study, nano-polycatenanes of variable length have been formed uncontrollably from the monomer that provides nanotoroids with sufficiently wide inner void space wherein secondary nucleation is driven by non-specific solvophobic interaction. In this study, we found that the elongation of the alkyl chain length of the barbiturate monomer decreases the inner void space of nanotoroids while increasing the frequency of secondary nucleation. These two effects resulted in an increase in the yield of nano-[2]catenane. This unique property observed in our self-assembled nanocatenanes might be extended to a controlled synthesis of covalent polycatenanes using non-specific interactions.
闭环超分子聚合与二次成核的明智结合,可以将带有3,4,5-三(十二烷氧基)苄氧基单元的二苯基萘巴比妥酸酯单体分层组织成由纳米环面组成的自组装纳米聚索烃。在我们之前的研究中,由提供具有足够宽内部空隙空间的纳米环面的单体不可控地形成了可变长度的纳米聚索烃,其中二次成核由非特异性疏溶剂相互作用驱动。在本研究中,我们发现巴比妥酸酯单体烷基链长度的延长会减小纳米环面的内部空隙空间,同时增加二次成核的频率。这两种效应导致纳米[2]索烃产率的提高。在我们的自组装纳米索烃中观察到的这种独特性质可能会扩展到使用非特异性相互作用对共价聚索烃进行的可控合成。