Structural modifications in carbon nitrides and related carbon-based materials have been achieved in recent years by organizing their monomers into versatile supramolecular structures that serve as reactants for the high temperature solid-state reaction. To date, the organization is usually carried out in one solvent where the building blocks must be dispersed. Here, we show the utilization of a molecule with both hydrogen bond donor and acceptor sites for constructing hydrogen bonded frameworks in interfacial systems. The chemical and electronic properties of the carbon nitride materials after calcination are strongly altered showing enhanced photocatalytic performance in different model reactions. This work shows a new large-scale pathway for the synthesis of highly photoactive carbon nitride with tailored properties and morphology by employing novel supramolecular assemblies prepared in the interface between two solvents, and furthermore opens new opportunities in the rational design of different carbon-nitrogen based materials utilizing supramolecular structures.
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