Room Temperature Self‐Healable Thermoplastic‐Elastomeric Blend Materials Based on Reversible Imine Bonded Cross‐Linked Polydimethylsiloxane Elastomer and Thermoplastic Polyurethane in Association With H‐Bonding and Their Characterization

Herein, both reversible covalent bonds (imine bond) and noncovalent interactions (H‐bonding) are incorporated into thermoplastic elastomeric blend materials to impart remarkable self‐healing properties at room temperature without any external stimuli. First, a Schiff base reaction occurs between amino‐functionalized polydimethylsiloxane (AFPDMS) and 1, 3, 5‐triformylbenzene (TFB), generating reversible imine‐bonded polydimethylsiloxane elastomer (CL‐PDMS), which is usually mechanically weak. Hence, thermoplastic polyurethane (TPU) is blended with it to obtain a blend material having good mechanical properties as well as room temperature healing ability. FTIR analysis confirmed both the presence of imine bonds in CL‐PDMS and hydrogen bonding between CL‐PDMS and TPU. The healing efficiency is dependent on the healing time and TFB content. Additionally, as the content of TPU in the blend increased, the healing efficiency and tensile properties correspondingly increased. The tensile strength of 200.7 kPa and elongation at break of 155.6% was observed for the CL‐PDMS/TPU (80/20) wt.% blend sample. This blend exhibited a maximum healing efficiency and recovered 98.7% and 96.4% of its original tensile strength and elongation‐at‐break, respectively, when healed at room temperature for 6 h. Moreover, graphene oxide was integrated with this polymer blend system to prepare self‐healing materials that may be used for flexible electronic devices.