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Structural adhesion at high temperature has been a challenge for organic adhesives, and the commercially available adhesives that can work at a temperature above 150 °C is rather limited. Herein, two novel polymers were designed and synthesized via facile strategy, which involves polymerization between melamine (M) and M-Xylylenediamine (X), as well as copolymerization of MX and urea (U). With well-balanced rigid-flexible structures, the obtained MX and MXU resins were proved to be outstanding structural adhesives at a wide range temperature of -196~200 °C. They provided room-temperature bonding strength of 13~27 MPa for various substrates, steel bonding strength of 17~18 MPa at cryogenic temperature (-196 °C), and 15~17 MPa at 150 °C. Remarkably, high bonding strength of 10~11 MPa was retained even at 200 °C. Such superior performances were attributed to a high content of aromatic units, which leads to high glass transition temperature (T g ) up to ~179 °C, as well as the structural flexibility endowed by the dispersed rotatable methylene linkages.

Tough Structural Adhesives with Ultra-Resistance to Both High and Cryogenic Temperature