Self-Healable and Recyclable Dual-Shape Memory Liquid Metal–Elastomer Composites

Liquid metal (LM)–polymer composites that combine the thermal and electrical conductivity of LMs with the shape-morphing capability of polymers are attracting a great deal of attention in the fields of reconfigurable electronics and soft robotics. However, investigation of the synergetic effect between the shape-changing properties of LMs and polymer matrices is lacking. Herein, a self-healable and recyclable dual-shape memory composite, comprising an LM (gallium) and a Diels–Alder (DA) crosslinked crystalline polyurethane (PU) elastomer, is reported. The composite exhibits a bilayer structure and achieves excellent shape programming abilities, due to the phase transitions of the LM and the crystalline PU elastomers. To demonstrate these shape-morphing abilities, a heat-triggered soft gripper, which can grasp and release objects according to the environmental temperature, is designed and built. Similarly, combining the electrical conductivity and the dual-shape memory effect of the composite, a light-controlled reconfigurable switch for a circuit is produced. In addition, due to the reversible nature of DA bonds, the composite is self-healable and recyclable. Both the LM and PU elastomer are recyclable, demonstrating the extremely high recycling efficiency (up to 96.7%) of the LM, as well as similar mechanical properties between the reprocessed elastomers and the pristine ones.