Yi-Ju WuYi-Hung LiuSheng-Hsien Chiu2024-10-242024-10-242024-07-27https://scholars.lib.ntu.edu.tw/handle/123456789/722385Herein we demonstrate an “in-ring establishing” strategy for assembling interlocked molecules through dynamic imine formation, “establishing” the host recognition sites in situ. Using Zn2+ ions to template the assembly of a pyridine-containing macrocycle with semidumbbell-shaped triazole-containing aldehyde and amine derivatives, we obtained the corresponding [2]rotaxane in high yield (85 %) after subsequent imine reduction (NaBH4) and amine protonation (NH4PF6). We performed the same three steps (assembly, reduction, protonation) to prepare a stable and highly symmetrical [5]molecular necklace ([5]MN) from 12 components (two almost-90°-oriented dialdehydes, two almost-90°-oriented diamines, four macrocycles, four Zn2+ ions) in an overall yield of 69 %.encatenanesdynamic covalent bondsiminesmolecular necklacesrotaxanes[SDGs]SDG3journal article10.1002/chem.202402404