Phase Segregation in Supramolecular Polymers Based on Telechelics Synthesized via Multicomponent Reactions

The properties of supramolecular polymers in the solid state are strongly dependent on the binding strength of the supramolecular motifs used; however, It has been previously shown that the nanostructure of supramolecular polymers plays an equally important role. Supramolecular polymers are commonly synthesized via end-group functionalization of low-glass transition telechelics with supramolecular units. In these systems, the binding motifs segregate from the soft telechelic backbone and form a hydrogen bonded crystalline hard phase that provides physical cross-links. To date, the reported synthetic approaches do not permit the introduction of a wide variety of supramolecular units with low synthetic effort, which would facilitate studying the structure-property relationships. The use of the Passerini and Ugi multicomponent reactions to synthesize various poly(ethylene-co-butylene) telechelics with diverse amide end-groups is reported. The thermal properties of the supramolecular polymers obtained through their solid-state assembly are investigated and their nanophase- segregation is studied, which is dictated by the end-group volume fraction and the amide–amide hydrogen bonding.