On-Surface Carbon Nitride Growth from Polymerization of 2,5,8-Triazido-s-heptazine

Carbon nitrides have recently come into focus for photo- and thermal catalysis, both as support materials for metal nanoparticles as well as photocatalysts themselves. While many approaches for the synthesis of three-dimensional carbon nitride materials are available, only top-down approaches by exfoliation of powders lead to thin-film flakes of this inherently two-dimensional material. Here, we describe an in situ on-surface synthesis of monolayer 2D carbon nitride films as a first step toward precise combination with other 2D materials. Starting with a single monomer precursor, we show that 2,5,8-triazido-s-heptazine can be evaporated intact, deposited on a single crystalline Au(111) or graphite support, and activated via azide decomposition and subsequent coupling to form a covalent polyheptazine network. We demonstrate that the activation can occur in three pathways, via electrons (X-ray illumination), via photons (UV illumination), and thermally. Our work paves the way to coat materials with extended carbon nitride networks that are, as we show, stable under ambient conditions.

Automated summary

Carbon nitrides have gained attention for their applications in both photo- and thermal catalysis. In this study, the authors describe an in situ method for synthesizing monolayer 2D carbon nitride films, which can be combined with other 2D materials. They show that a specific precursor can be evaporated, deposited, and activated to form a stable polyheptazine network using three pathways: electrons, photons, and thermal activation.