A General Synthesis Method for Covalent Organic Framework and Inorganic 2D Materials Hybrids.

Two-dimensional (2D) inorganic/organic hybrids provide a versatile platform for diverse applications, including electronic, catalysis, and energy storage devices. The recent surge in 2D covalent organic frameworks (COFs) has introduced an organic counterpart for the development of advanced 2D organic/inorganic hybrids with improved electronic coupling, charge separation, and carrier mobility. However, existing synthesis methods have primarily focused on few-layered film structures, which limits scalability for practical applications. Herein, we present a general synthesis approach for a range of COF/inorganic 2D material hybrids, utilizing 2D inorganic materials as both catalysts and inorganic building blocks. By leveraging the intrinsic Lewis acid sites on the inorganic 2D materials such as hexagonal boron nitride (hBN) and transition metal dichalcogenides, COFs with diverse functional groups and topologies can grow on the surface of inorganic 2D materials. The controlled 2D morphology and excellent solution dispersibility of the resulting hybrids allow for easy processing into films through vacuum filtration. As proof of concept, hBN/COF films were employed as filters for Rhodamine 6G removal under flow-through conditions, achieving a removal rate exceeding 93%. The present work provides a simple and versatile synthesis method for the scalable fabrication of COF/inorganic 2D hybrids, offering exciting opportunities for practical applications such as water treatment and energy storage.