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

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CHEMISTRY OF MATERIALS
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AMER CHEMICAL SOC
DOI: 10.1021/acs.chemmater.3c01030

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Carbon nitrides have gained attention as support materials for metal nanoparticles and as photocatalysts themselves. A new method has been developed to synthesize monolayer 2D carbon nitride films on a single crystalline support through in situ on-surface synthesis. The activation of the carbon nitride films can occur through three pathways: electrons, photons, and thermal energy. This work opens up possibilities for coating materials with stable carbon nitride networks under ambient conditions.
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.

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