Effect of bio-based epoxidized natural rubber as a compatibilizer in thermoplastic polyurethane/natural rubber blends: Physical characterization and 3D printing behavior

Thermoplastic natural rubber (TPNR) is widely used across industries due to its unique blend of elasticity and processability. Thermoplastic vulcanizates (TPVs) based on thermoplastic polyurethane (TPU) offer excellent mechanical properties and flexibility, yet often require enhanced elasticity and durability. Blending TPU with natural rubber (NR) is promising; however, phase incompatibility reduces mechanical strength and thermal stability. To address this, epoxidized NR (ENR) was employed as a compatibilizer in TPU/NR blends. ENR’s hydrocarbon backbone interacts with crosslinked NR, while epoxy groups enhance adhesion with TPU. Incorporating 3 phr of ENR significantly improved crosslinking, increased tensile strength by 41.1%, enhanced stress relaxation, and lowered the glass transition temperatures of both TPU and NR phases in the TPU/NR blends. These effects are attributed to improved chemical bridging between TPU and NR. However, excess ENR disrupts phase compatibility, causing polymer entanglement and reduced strength. Optimizing ENR content is essential for developing high-performance TPU/NR blends. Printability was demonstrated using the material extrusion additive manufacturing (MEx-AM) fused deposition modeling (FDM), showing potential for flexible applications like splints and medical devices.