Bio-Based, Self-Healing, Recyclable, Reconfigurable Multifunctional Polymers with Both One-Way and Two-Way Shape Memory Properties

Shape memory polymers (SMPs) have attracted wide attention over the past few decades due to their fantastic applications in modern life. Nevertheless, excellent self-healing properties, recyclability, solid-state plasticity, and reversible shape-switching ability are necessary but can rarely be satisfied in one material. Herein, we report multifunctional SMPs by constructing a dynamic boronic ester bond cross-linking network using sustainable Eucommia ulmoides gum as a raw material. Thanks to the crystallization and wide melting temperature range, these kinds of SMPs have thermal-triggered one-way shape memory performance and show two-way shape memory properties, whether under constant stress or stress-free conditions. Owing to the dynamic nature of the boronic ester bond, it exhibits good self-healing properties (near 100% at 80 °C), shape reconfigurability, and chemical recyclability. In addition, by incorporating multiwalled carbon nanotubes, the formed composite is responsive to 808 nm near-infrared light. Its applications are further exploited, including photoresponsive actuators, vascular stents, and light-driven switches. This paper provides a simple way for fabricating multifunctional SMPs, and the as-prepared materials have potential applications in diverse fields, such as biomedicine, intelligent sensing, and soft robotics.