Dual-Recyclable Biobased Elastomers with Hydrogen-Bonded Networks toward Sustainable Adhesives

In response to the demands of sustainable societal development, the integration of an excellent self-healing capability, adhesive property, recyclability, and desirable mechanical performance is crucial for the application of functional elastomers. In this work, we report a simple construction of a biobased elastomer from carboxylated tung oil polymer and phenolated lignin, which could offer reversible hydrogen bonding networks to achieve outstanding self-healability and dual recyclability. For instance, the biobased elastomer could be recycled rapidly under relatively mild conditions via hot-pressing or solvent-assisted methods, with only a slight decrease observed in its tensile strength. Meanwhile, the abundance of polar groups (especially catechol groups) within the elastomer enables good and reusable adhesion to a variety of substrates. In addition, the adhesion and mechanical properties of the biobased elastomers can be tailored by regulating their building block composition. This work provides an architectural design paradigm for functional elastomers that simultaneously integrate sustainability, self-healing, recyclability, and adhesion, making them suitable for emerging applications like advanced adhesives.