Soft-Rigid Construction of Mechanically Robust, Thermally Stable, and Self-Healing Polyimine Networks with Strongly Recyclable Adhesion

Author：Jia, Z. C., Wang, H. Y., Yu, P., He, H. F., Huang, Q. R., Hong, W., Liu, C., Shi, Y. J., Wang, J., Xin, Y. M., Jia, X. M., Ma, J. J., Yu, B.

Journal：Small

DOI:  10.1002/smll.202406821

Keywords: imidazole, polyimine networks, recyclable adhesion, recycling, self-healing, flame-retardant, Chemistry, Science & Technology - Other, Topics, Materials Science, Physics

Abstract: 

Reversible and recyclable thermosets have garnered increasing attention for their smart functionality and sustainability. However, they still face challenges in balancing comprehensive performance and dynamic features. Herein, silicon (Si)& horbar;oxygen (O) and imidazole units covalent bonds are coupled to generate a new class of bio-polyimines (Bio-Si-PABZs), to endow them with high performance and excellent reprocessing capability and acid-degradability. By tailoring the molar content of diamines, this Bio-Si-PABZs displayed both a markedly high glass transition temperature (162 degrees C) and a high char yield at 800 degrees C in an oxygen atmosphere (73.1%). These Bio-Si-PABZs with their favorable properties outperformed various previously reported polyimines and competed effectively with commercial fossil-based polycarbonate. Moreover, the scratch (approximate to 10 mu m) on the surface of samples can be self-healing within only 2 min, and an effective Bird Nest-to-Torch recycling can also be achieved through free amines solution. Most importantly, a bio-based siloxane adhesive derived from the intermediate Bio-Si-PABZ-1 by acidic degradation demonstrated broad and robust adhesion in various substrates, with values reaching up to approximate to 3.5 MPa. For the first time, this study lays the scientific groundwork for designing robust and recyclable polyimine thermosets with Si & horbar;O and imidazole units, as well as converting plastic wastes into thermal-reversibility and renewable adhesives. For the first time, by proposing a scheme to achieve high-performance bio-polyimines through optimizing the balance between silicon (Si)& horbar;oxygen (O) bonds and imidazole units, the field is advanced by reducing the acid concentration for the preparation of recycling bio-based adhesive. Moreover, the rare combination of strong interfacial bonding and enhanced cohesion via an elegant integration of Si & horbar;O bonding and pi-pi interactions. image