4.8 Article

Self-assembly of colloidal single-layer carbon nitride

Journal

NANOSCALE
Volume 14, Issue 34, Pages 12347-12357

Publisher

ROYAL SOC CHEMISTRY
DOI: 10.1039/d2nr03477h

Keywords

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Funding

  1. Deutsche Forschungsgemeinschaft (DFG) [ZA-146/45-1]
  2. Alexandr von Humboldt Foundation

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We propose a new concept of bottom-to-top design of intercalate carbon nitride compounds based on the self-assembly effects of colloidal single-layer carbon nitride (SLCN) sheets. The self-assembly includes the formation of intercalates of NEt4OH during the drying of SLCN colloids and the spontaneous formation of layered hexagonally-shaped networks on mica surfaces. The dynamics of intercalate formation were studied using in situ X-ray diffraction, and the structure of the intercalates was characterized by vibrational spectroscopy. The self-assembly on mica is driven by both the hexagonal symmetry of heptazine units and the templating effect of the mica surface.
We introduce a new concept of a bottom-to-top design of intercalate carbon nitride compounds based on the effects of self-assembly of colloidal single-layer carbon nitride (SLCN) sheets stabilized by tetraethylammonium hydroxide NEt4OH upon ambient drying of the water solvent. These effects include (i) formation of stage-1 intercalates of NEt4OH during the ambient drying of SLCN colloids on glass substrates and (ii) the spontaneous formation of layered hexagonally-shaped networks of SLCN sheets on freshly-cleaved mica surfaces. The dynamics of the intercalate formation was followed by in situ X-ray diffraction allowing different stages to be identified, including the deposition of a primary wet intercalate of hydrated NEt4OH and the gradual elimination of excessive water during its ambient drying. The intercalated NEt4+ cations show a specific flattened conformation allowing the dynamics of formation and structure of the intercalate to be probed by vibrational spectroscopies. The two-dimensional self-assembly on mica is assumed to be driven both by the internal hexagonal symmetry of heptazine units and by a templating effect of the mica surface.

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