Construction of Covalent Organic Frameworks via Three-Component One-Pot Strecker and Povarov Reactions.

Postsynthetic modification (PSM) has been demonstrated to be a powerful method for achieving new covalent organic frameworks (COFs) via single or multistep organic functional group transformation on established COF frameworks. PSM, however, might sometimes lead to collapse of the COF framework, decreases in crystallinity or low post-synthetic yield due to the inherent limit of solid-state synthesis. Herein we report, for the first time, a new synthetic strategy that can generate new COFs via multicomponent one-pot in situ reac-tions. In total, twelve α-aminonitrile- and quinoline-linked COFs with high crystallinity and permanent porosity are suc-cessfully achieved by three-component one-pot in situ Streck-er and Povarov reactions under solvothermal conditions in high yields. The obtained COFs feature the same structures as those obtained from the stepwise PSM approach on an estab-lished imine-linked COF. This in situ multicomponent assem-bly strategy, as a synthetic methodology parallel to PSM, might open a new route for constructing COFs that are not possible under PSM conditions.