Macroscopic Ultralight Aerogel Monoliths of Imine-based Covalent Organic Frameworks

The use of covalent organic frameworks (COFs) in practical applications demands shaping them into macroscopic objects, which remains challenging. Herein, we report a simple three-step method to produce COF aerogels, based on sol-gel transition, solvent-exchange, and supercritical CO₂ drying, in which 2D imine-based COF sheets link together to form hierarchical porous structures. The resultant COF aerogel monoliths have extremely low densities (ca. 0.02 g cm^-3 ), high porosity (total porosity values of ca. 99 %), and mechanically behave as elastic materials under a moderate strain (<25-35 %) but become plastic under greater strain. Moreover, these COF aerogels maintain the micro- and meso-porosity of their constituent COFs, and show excellent absorption capacity (e.g. toluene uptake: 32 g g^-1 ), with high removal efficiency (ca. 99 %). The same three-step method can be used to create functional composites of these COF aerogels with nanomaterials.