Superstrong Yet On‐Demand Debondable Polyolefin Adhesives by Leveraging Bioinspired Nucleobase Interactions

ABSTRACT Effective debonding of adhesives is of vital importance for advanced circular repair and recycling of valuable products, enabling the reclamation of materials and promoting sustainability. However, the tradeoff between strong adhesion and mild debonding substantially hinders the rapid development of new adhesives and limits their widespread applications. Herein, we develop a new class of superstrong yet mildly debondable polyolefin adhesives by leveraging the bioinspired multiple hydrogen bonds of nucleobases. By merging thymine functionalities into the flexible polyolefin backbone, the obtained thymine‐containing polyolefins exhibit remarkable properties such as high strength, excellent toughness, superior energy dissipation, and extraordinary adhesion. The optimized hydrophobic hydrogen bonding polyolefin adhesive exhibits robust cohesion and stable interfacial adhesion due to multiple hydrogen bonds, resulting in slow proton exchange with water. The unique features of the thymine‐containing adhesive enable us to achieve debonding under controlled and mild conditions. The debonding and rebonding cycles of the fragile and valuable silicon photovoltaic cells were carried out, demonstrating the robust yet on‐demand debondable properties of the adhesive. Overall, this work reports a bioinspired strategy to fabricate the ultrastrong but mildly detachable adhesive, which is poised to amplify advanced repair and recycling applications across various fields.