Heterogeneous Acrylic Resins with Bicontinuous Nanodomains as Low‐Modulus Flexible Adhesives

Abstract Adhesives play a critical role in the assembly of electronic devices, particularly as devices become more diverse in form factors. Flexible displays require highly transparent and rapidly recoverable adhesives with a certain stiffness. In this study, novel structured adhesives are developed that incorporate bicontinuous nanodomains to fabricate flexible adhesives with low moduli. This structure is obtained via polymerization‐induced microphase separation using a macro chain transfer agent (CTA). Phase separation is characterized using small‐angle X‐ray scattering, transmission electron microscopy, and dynamic mechanical analysis. By optimizing the length of the macro CTA, an adhesive with both hard and soft nanodomains is produced, resulting in exceptional flexibility (strain recovery = 93%) and minimal modulus (maximum stress/applied strain = 7 kPa), which overperforms traditional adhesives. The optimized adhesive exhibits excellent resilience under extensive strain, as well as strong adhesion and transparency. Furthermore, dynamic folding tests demonstrate the exceptional stability of the adhesive under various temperature and humidity conditions, which is attributed to its unique structure. In summary, the distinct bicontinuous phase structure confers excellent transparency, flexibility, and reduced stiffness to the adhesive, rendering it well‐suited for commercial foldable displays and suggesting potential applications in stretchable displays and wearable electronics.