Abstract:To address the demand in the field of smart materials for integrated self-healing and recyclable functionalities, this paper proposed a preparation strategy for self-healing and recyclable polyurethane materials featuring a triple dynamic network. Through the copolymerization of 2, 6-diaminopyridine ( DAP ), polytetrahydrofuran, isophorone diisocyanate, and hydroxyethyl hexahydrotriazine, combined with the introduction of ZnCl2 to construct pyridine-Zn2+ coordination bonds, the polyurethane composites (DAPPU-Znx ) with a triple dynamic network comprising coordination bonds, hydrogen bonds, and hexahydrotriazine rings was successfully fabricated. The chemical structure and dynamic network were confirmed by Fourier-transform infrared spectroscopy and X-ray photoelectron spectroscopy. Property investigations reveal that the coordination bonds effectively enhance the thermal stability and mechanical strength of the material. At a Zn2+/DAP mole ratio of 1/2, the corresponding DAPPU-Zn1/2 sample exhibits optimal performance:a 5% thermal decomposition temperature of 279.4 ℃, a tensile strength of 43.91 MPa, and a tensile strength recovery rate of 85.76% for the self-healed sample. This improved performance is primarily attributed to the synergistic effect between coordination bonds and multiple hydrogen bonds. Furthermore, the materials demonstrate great degradation responsiveness under acidic conditions, completely degrading within 96 min in a 1 mol/L phosphoric acid/ethanol mixed solution. The main degradation mechanism involves the cleavage of the triple dynamic bonds, urea bonds, and urethane structures. This study provides a novel strategy for developing intelligent polyurethane materials that integrate high mechanical strength, excellent self-healing capability, and acid-responsive degradation.