One-Pot Preparation of Double-Network Epoxy Vitrimers with High Performance, Recyclability, and Two-Stage Stress Relaxation
Yuetian Du, Dong Wang
Abstract
Although considerable progress has been made in developing different types of vitrimers, ongoing challenges remain in tuning their mechanical and rheological properties, self-healing, and adhesion. Here, we demonstrate a one-pot method to produce a novel double-network epoxy vitrimer using an aliphatic amine cross-linker with a siloxane covalent bond and an aromatic amine cross-linker with a disulfide covalent bond. When a controlled two-stage curing process is employed, the markedly different reactivities of aliphatic amine and aromatic amine with epoxy allow for sequential cross-linked network formation, leading to the development of a double network that incorporates two types of dynamic covalent bonds. As a result, the produced vitrimers exhibit controllable mechanical, thermal, and rheological properties, as well as recyclability. This is evidenced by a tensile strength as high as 72 MPa, while maintaining ∼10% elongation at break, a wide glass-transition temperature range from 91 to 171 °C, and an adjustable two-stage stress relaxation. These characteristics suggest opportunities to develop high-performance cross-linked polymers with specific responses to time and temperatures.