All-Ceramic and Elastic Aerogels with Nanofibrous-Granular Binary Synergistic Structure for Thermal Superinsulation

High-performance thermally insulating ceramic materials with robust mechanical properties, high-temperature resistance, and excellent thermal insulation characteristics are highly desirable for thermal management systems under extreme conditions. However, the large-scale application of traditional ceramic granular aerogels is still limited by their brittleness and stiff nature, while ceramic fibrous aerogels often display high thermal conductivity. To meet the above requirements, in this study, ceramic nanofibrous-granular composite aerogels with lamellar multiarch cellular structure and leaf-like fibrous-granular binary networks are designed and fabricated. The resulting composite aerogels possess ultralow weight, superelasticity with recoverable compression strain up to 80%, and large mechanical strength. Furthermore, excellent fatigue resistance with 1.2% plastic deformation after 1000 cyclic compressions, temperature-invariant dynamic mechanical stability from −100 to 500 °C, and an operational temperature range from −196 to 1100 °C are successfully achieved in the proposed composites. The nanosized silica granular aerogels are assembled into a leaf-like shape and wrapped around the fibrous cell walls, endowing low thermal conductivity (0.024 W m–1 K–1) as well as favorable high-temperature thermal superinsulation properties. Benefiting from the favorable compatibility, the present strategy for nanofiber-granular composite ceramic aerogels provides a dominant route to produce thermally insulated and mechanically robust composite cellular materials for use in harsh environments.