Architected Dual-Network Solvent-free Adhesives for Stretchable Fabrics

Abstract: Natural systems, such as tendons and spider silk, demonstrate how the combination of strength and stretchability can be effectively achieved by integrating stiff and flexible network structures. Inspired by these systems, we developed a novel, solvent-free dual-network adhesive based on a self-assembling ABA triblock copolymer, poly(methyl methacrylate)-poly(n-butyl acrylate)-poly(methyl methacrylate) (PMMA-b-PnBA-b-PMMA), designed for applications requiring both high strength and stretchability. The triblock copolymer forms a physically crosslinked network through microdomains of PMMA end-blocks that provide structural integrity, while the PnBA mid-block forms a soft, stretchable matrix. To further enhance mechanical performance, a second poly(n-butyl acrylate) (PnBA) network is polymerized in situ, locking the PMMA microdomains in place and creating a load-bearing system. By varying the crosslinking density of the secondary network, we tailor the adhesive's mechanical properties (Young's modulus: 0.17 - 1.18 MPa) to suit different substrates, creating a mechanically transparent seam. The resulting dual-network system combines different strategies to achieve high strength and stretchability, with adhesive performance comparable to industrial methods such as sewing, particularly in bonding neoprene fabric composites and sealing the joints. Our solvent-free approach also eliminates the need for lengthy solvent evaporation steps, offering an eco-friendly and more efficient alternative for flexible adhesive applications in fields such as soft robotics, flexible electronics, and sports apparel.