High‐performance vitrimer films containing acylhydrazone dynamic covalent bonds

Abstract Vitrimer films containing acylhydrazone bonds are synthesized in two steps. Bio‐based vanillin and adipate dihydrazide are used to prepare diols containing acylhydrazone bonds in one step, which are introduced into the reaction system of vitrimer to obtain the final films. The process is concise and easy to operate. By utilizing the rigid structure of vitrimer films and introducing dynamic acylhydrazone bonds, the obtained vitrimer films exhibit strong mechanical strength (maximum tensile strength of 27.10 MPa and maintaining up to 185.52% of the original breaking strength), excellent self‐healing property (tensile strength of 26.26 MPa after 12 h of primary self‐healing and 5.24 MPa after 12 h of secondary self‐healing), and rapid shape memory property (recovery time of about 2 min), strong acid and alkali resistance (not dissolved within 24 h), good thermal stability (no decomposition occurs below 160 °C), and high storage modulus (reaches 1087 MPa). These comprehensive benefits yield a certain reference for the preparation of vitrimer materials with prime properties.