From Millimeter to Subnanometer: Vapor–Solid Deposition of Carbon Nitride Hierarchical Nanostructures Directed by Supramolecular Assembly

Shape and nanostructure control has great potential to enable graphitic carbon nitride (C₃N₄) structures with new properties and functionalities. In this work, a new type of hierarchically structured nanoporous C₃N₄ is introduced. The C₃N₄ exhibits unique, edelweiss-like morphology, with components ranging from millimeter-sized bunches to subnanometer-thick layers. A one-step vapor–solid deposition approach using supramolecular aggregates as the precursor is carried out to accomplish the growth. Supramolecular pre-association plays a crucial role in achieving this nanostructure by directing the vaporization and deposition processes. Furthermore, very small C₃N₄ quantum dots can be readily acquired by bath sonication of the thin layers in water. The supramolecular preorganization growth strategy developed herein may provide a general methodology in the design of advanced photoelectric materials with broad applications in energy conversion and storage.