Supramolecular polymers based on 2-ureido-4[1H]-pyrimidone (UPy) units with extremely high dimerization constants and adjustable properties have received significant attention. In this work, we attempt to discuss the relationship between the micro-phase separation and the viscoelastic properties of the supramolecular polymers. For this reason, polymers with different UPy moieties structures and different UPy moieties contents were prepared and studied. It was found that the UPy moiety with little hindrance at the six-position of the pyrimidone could self-assemble into a nano-fiber structure and the degree of the micro-phase separation increased with the content of the UPy moiety. With the enlargement of the steric hindrance of the six-position of the pyrimidone, the nano-fiber structure gradually disappeared, meaning the degree of the micro-phase separation decreased astonishingly. More importantly, with the degree of the micro-phase separation increased, the storage modulus or the elasticity modulus increased exponentially and the T m and the loss modulus area increased linearly. These results would lead a new way to study and develop novel polymeric materials.
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