Development of tough and stiff elastomers by leveraging hydrophilic–hydrophobic supramolecular segment interaction

The presence of supramolecular interactions plays a crucial role in the formation of resilient multifunctional elastomers. Nevertheless, achieving elastomers with fabulous mechanical properties remains a significant challenge due to the incomplete understanding of the underlying principles. In this study, we have presented a simple yet efficient approach for manipulating the microstructure, resulting in a significant enhancement of the mechanical properties of the elastomers. By utilizing hydrophobic and hydrophilic extended chain segments to elongate a hydrophilic oligomer, we successfully created elastomers with improved toughness and stiffness through supramolecular interactions. The elastomer with hydrophobic extended chain segments demonstrates a fracture energy (94 842 J m^-2) and high tensile stress (16 MPa). In contrast, the elastomer with hydrophilic extended segments showed significantly lower tensile stress (0.18 MPa), even though their molecular chain structures are nearly identical. We conducted a systematic demonstration and investigation of the significant difference mentioned above and ultimately found that due to the hydrophobic-hydrophilic difference between the oligomer and extended chain segments, the hydrophobic chain segments are able to create hydrophobic association and the association can further facilitate the development of stronger and more abundant supramolecular interactions (hydrogen bonds). The resulting hydrogen bonds, combined with the hydrophobic association, effectively disperse energy and consequently improve the elastomer's capacity to withstand external forces. The hydrophilic-hydrophobic mechanism showcases the potential for creating durable supramolecular materials with promising applications in biology and electronics.