Mechanically robust and thermal-insulated polyimide aerogel films by polymerization-regulated strategy for flexible thermal protection

The development of flexible and foldable aerogels for thermal protection in harsh environments has been a long-term challenge as high porosity and weak interface connection can result in typical brittleness. Herein, a remarkable polymerization-regulated strategy was proposed to prepare polyimide (PI) aerogel films with high flexibility and efficient thermal insulation in extreme temperatures by using a facile phase-separation (PS-PI films) method. The polymerization degree of monomers was innovatively used to regulate the flexibility and mechanical properties of PS-PI films by slightly regulating the proportion of monomers. The results showed that the PI aerogel film realized the transition from brittleness to high flexibility, and the tensile strength and fracture strain of PS-PI films were increased by 3 times (11.7 MPa) and 4 times (18.7 %), respectively. Besides, a finite element model was established to analyze the tensile deformation process, revealing the destruction mechanism of aerogel film. The prepared PS-PI film also exhibited robust mechanical properties and efficient thermal insulation properties at extreme temperatures (−130 to 300 °C). The developed PS-PI film possessed high flexibility and efficient thermal-insulated performance at extreme temperatures, which could be a potential candidate for thermal protection in aerospace, energy, and buildings.