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High-Performance,Light-Stimulation Healable,and Closed-Loop Recyclable Lignin-Based Covalent Adaptable Networks
Authors:Xiaozhen Ma  Xiaolin Wang  Honglong Zhao  Xiaobo Xu  Minghui Cui  Nathan E Stott  Peng Chen  Jin Zhu  Ning Yan  Jing Chen
Affiliation:1. Key Laboratory of Bio-based Polymeric Materials Technology and Application of Zhejiang Province, Laboratory of Polymers and Composites, Ningbo Institute of Materials Technology and Engineering, Chinese Academy of Sciences, Ningbo, 315201 China

University of Chinese Academy of Sciences, Beijing, 100039 China;2. Key Laboratory of Bio-based Polymeric Materials Technology and Application of Zhejiang Province, Laboratory of Polymers and Composites, Ningbo Institute of Materials Technology and Engineering, Chinese Academy of Sciences, Ningbo, 315201 China;3. Key Laboratory of Bio-based Polymeric Materials Technology and Application of Zhejiang Province, Laboratory of Polymers and Composites, Ningbo Institute of Materials Technology and Engineering, Chinese Academy of Sciences, Ningbo, 315201 China

School of Materials Science and Chemical Engineering, Ningbo University, Ningbo, Zhejiang, 315211 China;4. Key Laboratory of Bio-based Polymeric Materials Technology and Application of Zhejiang Province, Laboratory of Polymers and Composites, Ningbo Institute of Materials Technology and Engineering, Chinese Academy of Sciences, Ningbo, 315201 China

School of Materials Science and Engineering, Shenyang University of Chemical Technology, Shenyang, Liaoning, 110142 China;5. Department of Chemical Engineering and Applied Chemistry, University of Toronto, Toronto, Ontario, M5S 3E5 Canada

Abstract: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.
Keywords:closed-loop recovery  high performance  light-controlled healable  unmodified lignin  Zn2+ coordination bonds
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