A General Group-Protection Synthesis Strategy to Fabricate Covalent Organic Framework Gels

Fabricating insoluble and infusible porous materials into gels for advanced applications is of great importance but has formidable challenges. Here, we present a general, facile, and scalable protocol to fabricate covalent organic framework (COF) gels using a group-protection synthesis strategy. To prove the generality of this strategy, we successfully prepared 10 types of COF organohydrogels with high crystallinity, porosity, good mechanical properties, and excellent solvent and freezing resistance. Notably, these COF organohydrogels can easily transform into hydrogels, organogels, and aerogels, breaking the gaps between different types of COF gels. An in-depth mechanism investigation unveils that the group-protection strategy effectively slows down the formation rate and regulates the morphology of COFs, benefiting the formation of cross-linked nanofibers/nanosheets to produce COF gels. We also find that the hydrogen bond network formed by the organic/water binary solvent and functional groups in the COF skeletons plays a vital role in creating organohydrogels and maintaining frost resistance and solvent resistance. As an application demonstration, COF gels installed with photoresponsive azobenzene groups show excellent solar energy absorption, photothermal conversion, and water transmission performances, demonstrating great potential in solar desalination. This work enriches the synthesis toolboxes for COF gels and expands the application scope of COFs.