Mechanically strong, healable, and recyclable supramolecular solid–solid phase change materials with high thermal conductivity for thermal energy storage

•Mechanically strong, healable, and recyclable supramolecular SSPCMs were synthesized.•The supramolecular SSPCMs retained excellent energy storage capacity and thermal shape memory.•The solar thermal composite with highly directional thermal conductivity contributed to rapid solar thermal conversion and storage. Conventional polymeric solid–solid phase change materials (SSPCMs) have garnered significant attention in the development of state-of-the-art latent heat storage (LHS) systems. However, the industrial application of polymeric SSPCMs is compromised by inferior mechanical properties and intrinsic low thermal conductivity. In addition, they are unable to be recycled and self-healed due to permanently cross-linked structures. In this study, a series of healable and recyclable supramolecular SSPCMs (PEG4K-Bx-PEG6K), possessing robust tensile strength (∼22.90 MPa), excellent strain-at-break (∼733.62 %), and high toughness (∼120.05 MJ/m3), are designed and developed by incorporating dynamic boroxines and hydrogen bonds. Because of the reversibility of dynamic boroxines and hydrogen bonds, the PEG4K-Bx-PEG6K was able to be healable and conveniently processed into packaging bag. More importantly, the PEG4K-Bx-PEG6K also possessed high thermal storage capacity (98.03 J/g), and excellent thermal shape memory capability. To achieve efficient heat transfer, an orientated solar thermal composite with high thermal conductivity was fabricated by compression-induced repetitive stacking of oriented graphene nanosheets (GNs) layers in PEG4K-Bx-PEG6K. Thanks to the efficient heat conduction of oriented GNs layers in the composite, the directional thermal conductivity of composite was up to 3.639 W/mK at 5 wt% loading of GNs. Combining the above excellent heat conduction, the solar thermal composite developed in this work offered efficient solar thermal conversion, fast transportation and storage of the harvested thermal energy.