High‐Strength Recyclable Adhesives With Thermo‐ and Electro‐Triggered Debonding Derived From Sustainable Monomers

ABSTRACT The development of high‐strength, on‐demand debondable, and recyclable adhesives from renewable resources remains a major challenge. Herein, we present a facile strategy to construct robust, low‐molecular‐weight adhesives with thermally and electrically triggered debonding from sustainably sourced tannic acid and DL‐carnitine hydrochloride. The adhesive exhibits outstanding adhesion on various substrates, with a maximum adhesion strength of 14.4 MPa on ceramics. This superior strength originates from dense interaction sites and rich noncovalent interactions, which facilitate the multidimensional synergistic enhancement of both cohesive and adhesive energies. Notably, ionic moieties reorganize the hydrogen‐bond network, generating additional interfacial donors and acceptors that strengthen substrate adhesion. Remarkably, the adhesive allows for on‐demand debonding either thermally (75°C) or electrochemically (10 V, 60 s), triggered by the disruption of noncovalent interactions and oxidation of catechol or pyrogallol to quinone, respectively. Moreover, the adhesive can be recovered by water immersion, and the monomers can be efficiently separated and recovered via ethanol treatment. This work proposes a novel strategy for regulating adhesion performance via ionic moieties and establishes a new paradigm for triggered debonding through electrochemical oxidation.