Tailoring carbon nitride properties and photoactivity by interfacial engineering of hydrogen-bonded frameworks

The rational synthesis of carbon nitride materials, ranging from polymeric carbon nitride to nitrogen-doped carbon, by supramolecular preorganization of their monomers is a powerful tool for the design of their morphology and photophysical and catalytic activities. Here we show a new facile and scalable approach for the synthesis of ordered CN materials with excellent photoactivity, which consists of supramolecular interfacial preorganization of CN monomers at the interface of two non-miscible solvents. Molecular dynamic simulations supported by experimental results reveal that an appropriate choice of monomers and solvents leads to the formation of a supramolecular assembly solely at the interface of the solvents. As a proof of concept, we show that the properties of the CN materials after thermal condensation can be tuned by adding an additional monomer to one solvent only. The advantages of the new method are demonstrated here through the tunable morphologies and surface area, the formation of new electronic junctions and high activity as a photocatalyst for hydrogen evolution and pollutant degradation of the CN materials.