Ambient Construction of Quinazoline-Linked Covalent Organic Frameworks via Solar-Driven Intrinsic Photochemical Aromatization

Although solar-driven organic synthesis is highly attractive, its application in materials synthesis is still in its infancy and faces great challenges. Herein, we present the first sunlight-driven, photosensitizer-free strategy for constructing quinazoline-linked covalent organic frameworks (QZCOFs) via photochemical aromatization under ambient conditions. This approach enables the scalable synthesis of highly crystalline and robust QZCOFs featuring well-defined conjugated structures. The resulting QZCOF-1 possesses a donor–acceptor (D–A) architecture and serves as an efficient, metal-free heterogeneous photocatalyst for diverse organic transformations, including selective sulfide oxidation, benzimidazole formation, and tetrahydroquinoline synthesis via C–H annulation. This strategy not only opens a promising paradigm for the green and sustainable synthesis of COFs but also demonstrates their potential as multifunctional platforms for photocatalysis.