Towards Sustainable and Fire‐Safe Thermosets Using Phosphorus‐Containing Covalent Adaptable Networks

Abstract Dynamic covalent chemistry is a promising strategy for developing recyclable thermosets and their carbon fiber reinforced composites, in line with the goal of green and sustainable development. However, a significant challenge lies in balancing the dynamic reversibility and the desired service performances, such as thermal, mechanical properties, and flame retardancy. It has hindered the broader application of dynamic materials beyond the initial proof of concept. This concept provides an overview of the current state of research on phosphorus‐containing covalent adaptable networks (CANs), highlighting key designing and regulating principles for tailoring comprehensive properties including flame retardancy, mechanical and thermal properties, as well as dynamic behaviours such as malleability, reprocessability and degradability. Finally, new frontiers and opportunities in developing high‐performance sustainable CANs‐based thermosets and their carbon fiber composites for structural engineering applications are prospected.