Supramolecular/Dynamic Covalent Design of High‐Performance Pressure‐Sensitive Adhesive from Natural Low‐Molecular‐Weight Compounds

Adhesive materials have played an essential role in the history of humanity. Natural adhesives composed of low-molecular-weight monomers have been overshadowed by modern petroleum-based glues. With the development of green economy, the demand for eco-friendly materials has increased. Herein, two natural biocompatible compounds, namely thioctic acid (TA) and malic acid (MA), are selected to prepare a high-performance pressure-sensitive adhesive poly[TA-MA]. This adhesive can be quantitatively obtained via a simple mixing and heating process. Poly[TA-MA] shows interesting and useful properties, including reversible flexibility, high elongation, and good self-healing, owing to its dynamic polymerization pattern and reversible cross-linking behavior. Poly[TA-MA] exhibits excellent adhesion performance under various extreme conditions, such as at low temperatures and in hot water. High values of shear strength (3.86 MPa), peel strength (7.90 N cm^-1), loop tack (10.60 N cm^-1), tensile strength (1.02 MPa), and shear resistance (1628 h) demonstrate the strong adhesive effect of poly[TA-MA]. Additionally, TA can be regenerated in the monomer forms from poly[TA-MA] with high recovery rate (>90%). Meanwhile, strong anti-bacterial behavior of poly[TA-MA] is recorded. This study not only reported a new pressure-sensitive adhesive but also fully displayed the feasibility of using natural small molecules to achieve robust surface adhesion.