Supramolecular rubbers incorporating a large number of physical cross-links through cooperative hydrogen bonds display high self-healing properties but limited solvent and creep resistance due to the lack of chemical cross-links. Increasing both chemical cross-links and H-bonding is therefore desirable but limited by the functionality of monomers. The present work thus devises a convergent chemical platform permitting to increase the number of chemical cross-links without changing the concentration of hydrogen-bonding groups. Starting from a single reactive prepolymer, functionalized with a defined number of hydrogen-bonding groups, a series of networks presenting different ratios of diepoxide and tetraepoxide were prepared. The curing process (controlled by 2-MI catalyst), thermomechanical behavior, and tensile properties recovery of the cured materials were investigated. Gelation state was quantified and compared to theoretical predictions. The introduction of tetrafunctional epoxide in the presence of 2-MI gave rise to gelled materials characterized by higher rigidity and strength and significantly improved creep resistance. Self-healing was observed for all materials, with 50% to 100% complete recovery in a day depending on tetraepoxide content.

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Although the petrochemical polymers have revolutionized the technological development, the intensive use of these materials have contributed to the global pollution. In this context, researches involving ecofriendliness materials are growing up, as well as, a current interest in developing materials from inexpensive and renewable resources, such as vegetable oils. In this work, is described the synthesis of polymeric materials by thermal polymerization from linseed oil (Linum usitatissimum L.) and passion fruit oil (Passiflora edulis) and their characterization by gas chromatographic (GC), Fourier transform infrared (FTIR) spectroscopy, solubility in organic solvents, thermogravimetry (TG), differential scanning calorimetry (DSC) and Raman spectroscopy. The TG curve shows that those polymeric materials present two stages of decomposition. DSC plots of the vegetable oils showed some endothermic and exothermic transitions which are not present in the DSC curves corresponding to oil‐based polymers. The Raman spectra of the polymers indicate declining of absorbance in the region of CC stretching (∼1600 cm−1). This absorption was used to estimate the degree of polymerization (79% and 67.5% for linseed and passion fruit oils, respectively).