Recyclability and self-healing in biobased vitrimers: current progress and the role of 2D nanomaterial integration
摘要
Biobased vitrimers, a type of Covalent Adaptable Networks (CANs), present an innovative strategy for creating recyclable thermosetting polymers by integrating renewable resources with dynamic covalent bonding. This review compiles insights from many systems employing transesterification, imine exchange, disulfide metathesis, boronic ester metathesis, and phenol–carbamate exchange, emphasizing their self-healing, recyclability, and sustainability profiles. Key performance metrics such as topology freezing temperature (Tv), relaxation time (τ*), and healing efficiency (ηₕ) are analysed across vitrimer chemistries, with catalyst-free systems often achieving over 90% mechanical recovery and recyclability under mild conditions. A novel classification is introduced for recyclability strategies, covering thermal reprocessing, chemical depolymerization, and ambient self-healing. Special emphasis is placed on biobased sources like vanillin, lignin, soybean oil, and cardanol, which enable both sustainability and functionality. In addition, a dedicated section explores recent integrations of two-dimensional (2D) nanofillers such as carbon nanotubes (CNTs), graphene, MXenes, cellulose nanocrystals, and boron nitride into vitrimer matrices. These nanocomposites offer enhanced mechanical, thermal, and electrical properties while preserving recyclability and healing. However, only a few such systems fully incorporate biobased matrices, leaving ample room for further development.
Graphical abstract