High‐Performance, Light‐Stimulation Healable, and Closed‐Loop Recyclable Lignin‐Based Covalent Adaptable Networks

In this work, high-performance, light-stimulation healable, and closed-loop recyclable covalent adaptable networks are successfully synthesized from natural lignin-based polyurethane (LPU) Zn²⁺ coordination structures (LPUxZy). Using an optimized LPU (LPU-20 with a tensile strength of 28.4 ± 3.5 MPa) as the matrix for Zn²⁺ coordination, LPUs with covalent adaptable coordination networks are obtained that have different amounts of Zn. When the feed amount of ZnCl₂ is 9 wt%, the strength of LPU-20Z9 reaches 37.3 ± 3.1 MPa with a toughness of 175.4 ± 4.6 MJ m^-3 , which is 1.7 times of that of LPU-20. In addition, Zn²⁺ has a crucial catalytic effect on "dissociation mechanism" in the exchange reaction of LPU. Moreover, the Zn²⁺ -based coordination bonds significantly enhance the photothermal conversion capability of lignin. The maximum surface temperature of LPU-20Z9 reaches 118 °C under the near-infrared illumination of 0.8 W m^-2 . This allows the LPU-20Z9 to self-heal within 10 min. Due to the catalytic effect of Zn²⁺ , LPU-20Z9 can be degraded and recovered in ethanol completely. Through the investigation of the mechanisms for exchange reaction and the design of the closed-loop recycling method, this work is expected to provide insight into the development of novel LPUs with high-performance, light-stimulated heal ability, and closed-loop recyclability; which can be applied toward the expanded development of intelligent elastomers.