Synthesis of Crystalline Covalent Organic Frameworks Crosslinked through Hydrogen Bonding

Abstract Covalent organic frameworks crosslinked through hydrogen bonding (HcCOFs) exhibit considerable potential in combining the advantages of the stability of the covalent bonds with the flexibility and reversibility of the hydrogen bonds, creating a unique platform for assembling organic units into crystalline porous materials with unique properties and functions. In this work, a new crystalline HcCOF material is successfully synthesized for the first time via Schiff's base reaction and carboxylic acid self‐assembly. This material exhibits a response to humidity and efficient atmospheric water‐harvesting capabilities, showcasing its potential in materials science and providing a new path for future innovations in gas storage, catalysis, sensors, drug delivery, etc.