Development of Bio-Based and Recyclable Epoxy Adhesives by Modification with Thermoplastic Polymers

Abstract

This paper deals with the design of novel epoxy adhesives by incorporating thermoplastic polymers such as polyetherimide (PEI) and poly(ε-caprolactone) (PCL) into a bio-based and recyclable epoxy resin, known as Polar Bear. The adhesives were characterized by their mechanical (quasi-static and dynamic) and rheological properties, thermal stability, and adhesion properties in single-lap joints tested at three different temperatures (i.e., −55 °C, 23 °C, 80 °C). The experimental results indicated that low PEI content substantially improved the mechanical performance and toughness of the adhesive, while preserving good processability. Nonetheless, exceeding 3% weight percentage adversely affected the adhesives’ mechanical resistance and workability. Conversely, while PCL addition enhanced the adhesives’ viscosity, it also decreased mechanical performance. However, its eco-friendliness offers potential for sustainable adhesive applications. It is worth noting that regardless of temperature, the modified adhesives consistently outperformed the commercial epoxy adhesive (DP-460), used as reference, in single-lap shear joint tests. Additionally, both PEI- and PCL-modified epoxy adhesives have demonstrated recyclability through a simple acid-based process, enabling joint disassembly and recycling of the adhesive into a thermoplastic polymer. Overall, the modified adhesives represent a promising eco-friendly, high-performance alternative for structural applications, aligning with sustainable and circular practices.