Multifunctional Vitrimer-Like Polydimethylsiloxane (PDMS): Recyclable, Self-Healable, and Water-Driven Malleable Covalent Networks Based on Dynamic Imine Bond

Vitrimer is a new class of polymeric materials which can be reprocessed to any shape while being permanently cross-linked. We designed and synthesized a catalyst-free network with poly(dimethylsiloxane)etherimide (PDMS-NH2), terephthalaldehyde (TA), and tri(2-aminoethyl)amine (TREA) through the condensation reaction between amino groups and aldehyde groups. As a result of the exchange reaction of the dynamic imine bond obtained, this PDMS network exhibits the nature of vitrimer-like material, which is examined by solubility and stress-relaxation experiments, and the relaxation time is as short as 64 s at 130 °C. In addition, the vitrimer-like PDMS is malleable and capable of self-healing, and the mechanical properties can be maintained even after three consecutive breaking/mold pressing cycles. Especially, besides heating, this vitrimer-like PDMS can also be recycled and reshaped at ambient temperature due to the exchange reaction of dynamic imine bond when immersed in water, which will potentially lead t...