Dynamic Boronic Ester Cross-Linked Polymers with Tunable Properties via Side-Group Engineering.

The development of dynamic covalent materials with repairability, reprocessability, and recyclability is crucial for sustainable development. In this work, we report a new strategy to adjust the thermomechanical properties of boronic ester cross-linked poly(β-hydroxyl amine)s through side-group engineering. By tuning the side groups of the poly(β-hydroxyl amine)s, we have developed self-healable, reprocessable, and shape-programmable materials. By tuning the side groups of the poly(β-hydroxyl amine)s, the thermomechanical properties can be readily adjusted. Notably, the 3-amino-1,2-propanediol-derived polymer exhibits enhanced thermal (T = 95 °C) and mechanical (tensile strength = 34.2 MPa) performance due to increased hydrogen bonding. Benefiting from the dynamic reversibility of the boronic esters, these materials demonstrate solvent-assisted healing, reprocessing, chemical recycling, and shape programming capabilities. Given their straightforward synthesis, tunable properties, and robust dynamic features, the boronic ester cross-linked poly(β-hydroxyl amine)s hold great promise for various applications, including flexible electronic and biomedical materials.