Abstract

• Unidirectional anisotropic PIAs have been prepared by freeze-drying. • The PIA shows excellent thermal stability and stable mechanical behavior. • The u -PIA-6 exhibits great strength, which is over twice as high as that of the TEEK-HH at 177 °C with a similar density. • The u -PIA shows great thermal insulation properties in anisotropic. Polyimide aerogels (PIAs) are the new type of high-performance lightweight material that combines the excellent thermal and mechanical behavior of polyimides with the highly porous and lightweight properties of aerogels. PIAs can meet the increasing material requirements of high-tech fields such as the aerospace and transportation industries. This study reports a series of all-aromatic anisotropic polyimide aerogels (p-phenylenediamine (PDA) and 3,3′,4,4′-biphenyltetracarboxylic dianhydride (s-BPDA)) with unprecedented behavior. These PIAs were synthesized using a random or unidirectional freeze-drying method followed by thermal imidization of the precursor solution. Their mechanical and thermal conductivity performance were anisotropic ( u -PIA-8 strength: 1.86 and 0.14 MPa, thermal conductivity: 62.9 and 50.1 mW·m −1 ·K −1 along the axial and radial direction, respectively). Furthermore, the PIAs possessed excellent compression behavior in a wide temperature range from 25 °C to 316 °C, with a compressive strength over twice that of the commercial polyimide foam TEEK-HH ( u -PIA-6 strength: 0.83 and 0.32 MPa at 177 and 316 °C, TEEK-HH strength: 0.31 MPa at 177 °C). These aerogels also demonstrated good thermal insulation performance after being held at 300 °C for 20 min ( u -PIA-8: 76.3 °C at 25 mm). These highly anisotropic aerogels exhibit flexible thermal protection properties that extend the potential use of PIAs to applications such as high-temperature-resistant rocket fairings, sandwich structures, and arc-shaped structures for aerobats or the automobile industry.

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