We describe here a new process for the synthesis of very high quality 2D Covalent Organic Frameworks (COFs), such a C2N and CN carbon nitrides. This process relies on the use of a metallic surface as both a reagent and a support for the coupling of small halogenated building blocks. The conditions of the assembly reaction are chosen so as to leave the inorganic salts by-products on the surface, to further confine the assembly reaction on the surface and increase the quality of the 2D layers. We found that under these conditions, the process directly returns few layers material. The structure/quality of these materials is demonstrated by extensive cross-characterizations at different scales, combining optical microscopy, Scanning Electron Microscopy (SEM)/Transmission Electron Microscopy (TEM) and Energy Dispersive Spectroscopy (EDS). The availability of such very large, high-quality layers of these materials opens interesting perspectives, for example in photochemistry and electronics (intrinsic transport properties, high gap substrate for graphene, etc...).
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