Intrinsic Flame Retardancy and Flexible Solid–Solid Phase Change Materials with Self-Healing and Recyclability

Conventional polymeric phase change materials (PCMs) have been widely used due to their high heat storage density, small temperature variation, and nontoxicity. However, the high flammability and unrecyclable problems restrict their applications in energy storage devices (ESDs). Although it is facile to introduce a flame retardant into phase change materials to improve fire resistance, the physical blending will deteriorate the mechanical performance and thermal stability of PCMs. Herein, flame-retardant solid–solid PCMs (FRPCMs) with intrinsic flame retardancy, phase change property, self-healing, and recyclability were synthesized by simultaneously integrating tetrabromobisphenol A (TBBPA) and poly(ethylene glycol) (PEG) into polyurethane network skeletons. PEG ingredients acted as phase change materials, and TBBPA not only worked as an efficient flame retardant but also provided dynamic covalent bonds for thermally induced self-healing and recyclability. FRPCMs possess the highest latent heat of 124.7 J/g, high self-healing ability, and high thermal reliability and recyclability. Besides, with the introduction of TBBPA, the limiting oxygen index (LOI) value and char residue significantly increased, the heat release rate (HRR) and total heat release (THR) values decreased, and most of the FRPCMs reached UL94 V-2 rating as well. Hence, the synthesized FRPCMs could expand the application scope of PCMs for thermal energy storage.