Exploring the Role of Supramolecular Associations in Mechanical Toughening of Interpenetrating Polymer Networks

Abstract

Model “supramolecular IPNs” were developed via the formation of a hydrogen-bonded, supramolecular network of 2-ureido-4-[1H]-pyrimidinone (UPy) telechelic poly(ethylene-co-1-butene) (SPEB) in the presence of photopolymerizable, hydroxyl-terminated polybutadiene (HTPB). The role of a supramolecular elastomeric phase in mechanical toughening of IPNs was explored through (1) dynamic dissociation and reassociation of the noncovalent, UPy supramolecular associations, and (2) interphase formation. While an ∼4× increase in tensile toughness of the HTPB matrix was observed through incorporation of 10 wt % ethylene–propylene rubber (EPR)—as a conventional elastomeric toughening agent—into HTPB, it was shown that adding the same amount of supramolecular elastomer SPEB to HTPB led to ∼600× enhancement in tensile toughness. Strain rate-dependent mechanical response and fractography studies revealed that this dramatic toughness enhancement was due to dissociation/reassociation of the dynamic UPy linkages in the elasto...