Super-elasticity at 4 K of covalently crosslinked polyimide aerogels with negative Poisson's ratio

The deep cryogenic temperatures encountered in aerospace present significant challenges for the performance of elastic materials in spacecraft and related apparatus. Reported elastic carbon or ceramic aerogels overcome the low-temperature brittleness in conventional elastic polymers. However, complicated fabrication process and high costs greatly limited their applications. In this work, super-elasticity at a deep cryogenic temperature of covalently crosslinked polyimide (PI) aerogels is achieved based on scalable and low-cost directional dimethyl sulfoxide crystals assisted freeze gelation and freeze-drying strategy. The covalently crosslinked chemical structure, cellular architecture, negative Poisson's ratio (-0.2), low volume shrinkage (3.1%), and ultralow density (6.1 mg/cm³) endow the PI aerogels with an elastic compressive strain up to 99% even in liquid helium (4 K), almost zero loss of resilience after dramatic thermal shocks (∆T = 569 K), and fatigue resistance over 5000 times compressive cycles. This work provides a new pathway for constructing polymer-based materials with super-elasticity at deep cryogenic temperature, demonstrating much promise for extensive applications in ongoing and near-future aerospace exploration.