Fabricating High Strength Bio-Based Dynamic Networks from Epoxidized Soybean Oil and Poly(Butylene Adipate-co-Terephthalate)

Amid the rapid development of modern society, the widespread use of plastic products has led to significant environmental issues, including the accumulation of non-degradable waste and extensive consumption of non-renewable resources. Developing healable, recyclable, bio-based materials from abundant renewable resources using diverse dynamic interactions attracts increasing global attention. However, achieving a good balance between the self-healing capacity and mechanical performance, such as strength and toughness, remains challenging. In our study, we address this challenge by developing a new type of dynamic network from epoxidized soybean oil (ESO) and poly(butylene adipate-<i>co</i>-terephthalate) (PBAT) with good strength and toughness. For the synthetic strategy, a thiol-epoxy click reaction was conducted to functionalize ESO with thiol and hydroxyl groups. Subsequently, a curing reaction with isocyanates generated dynamic thiourethane and urethane bonds with different bonding energies in the dynamic networks to reach a trade-off between dynamic features and mechanical properties; amongst these, the thiourethane bonds with a lower bonding energy provide good dynamic features, while the urethane bonds with a higher bonding energy ensure good mechanical properties. The incorporation of flexible PBAT segments to form the rational multi-phase structure with crystalline domains further enhanced the products. A typical sample, OTSO₁₀₀-PBAT₁₀₀, exhibited a tensile strength of 33.2 MPa and an elongation at break of 1238%, demonstrating good healing capacity and desirable mechanical performance. This study provides a promising solution to contemporary environmental and energy challenges by developing materials that combine mechanical and repair properties. It addresses the specific gap of achieving a trade-off between tensile strength and elongation at break in bio-based self-healing materials, promising a wide range of applications.