Highly Stretchable yet Degradable and Recyclable Conductive Composites with Liquid Metal Nanodroplets as Physical Crosslinks

Liquid metal (LM) droplet‐embedded polymer composites with exceptional thermal, electrical, and mechanical characteristics are attractive for applications in soft electronics and thermal management. Generally, a high volume fraction of LMs is required for desirable thermal and electrical properties, and thus recycling of LMs is favorable and cost effective. However, recycling LMs from composites remains a formidable challenge because the LM droplets are typically dispersed into a permanent covalently crosslinked polymer matrix. Here, a facile synthesis of LM‐polymer composites with high electrical conductivity (1800 S cm−1), high stretchability (1400% tensile strain), as well as degradability and recyclability is reported. The composite comprises a poly(2‐hydroxyethyl acrylate) hydrogel that is physically crosslinked by LM nanodroplets as a polymer matrix and either LM microdroplets or silver microflakes as a conductive filler. A postdrying process improves the mechanical performance of the composite while creating percolating pathways via the rearrangement of the conductive fillers, imparting high electrical conductivity to the composite. Moreover, the composites are readily degraded and dissolved in aqueous alkali solutions at room temperature thanks to the reactive nature of LM crosslinks, enabling high recycling efficiency of ≈80% and 95% for composites with LM microdroplets and silver microflakes as conductive fillers, respectively. A composite hydrogel is synthesized with liquid metal (LM) nanodroplets as physical crosslinks as well as LM microdroplets or silver microflakes as conductive fillers. Dehydration of the composite hydrogel leads to mechanical enhancement and formation of percolating network and thus a dry composite that has high conductivity, high stretchability, degradability, and recyclability is obtained.