Exploring the evolution patterns of melem from thermal synthesis of melamine to graphitic carbon nitride† † Electronic supplementary information (ESI) available. See https://doi.org/10.1039/d2ra03337b
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ABSTRACT:
SUBMITTER: Yi Y
PROVIDER: S-EPMC9412154 | biostudies-literature | 2022 Aug
REPOSITORIES: biostudies-literature
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Project description:Melamine is a precursor and building block for graphitic carbon nitride (g-CN) materials, a group of layered materials showing great promise for catalytic applications. The synthetic pathway to g-CN includes a polycondensation reaction of melamine by evaporation of ammonia. Melamine molecules in the crystal organize into wave-like planes with an interlayer distance of 3.3 Å similar to that of g-CN. Here we present an extensive investigation of the experimental electron density of melamine obtained from modelling of synchrotron radiation X-ray single-crystal diffraction data measured at 25 K with special focus on the molecular geometry and intermolecular interactions. Both intra- and interlayer structures are dominated by hydrogen bonding and π-interactions. Theoretical gas-phase optimizations of the experimental molecular geometry show that bond lengths and angles for atoms in the same chemical environment (C-N bonds in the ring, amine groups) differ significantly more for the experimental geometry than for the gas-phase-optimized geometries, indicating that intermolecular interactions in the crystal affects the molecular geometry. In the experimental crystal geometry, one amine group has significantly more sp3 -like character than the others, hinting at a possible formation mechanism of g-CN. Topological analysis and energy frameworks show that the nitrogen atom in this amine group participates in weak intralayer hydrogen bonding. We hypothesize that melamine condenses to g-CN within the layers and that the unique amine group plays a key role in the condensation process.
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Project description:Graphitic carbon nitride (CN) was synthesized from guanidine hydrochloride (G), melamine (M) and dicyandiamide (DCDA). The CN materials synthetized from the pure precursors and their mixtures were characterized by common methods, including thermal analysis, and their photocatalytic activities were tested by the degradation of selected organic pollutants, such as amoxicillin, phenol, Rhodamine B (RhB). Remarkable changes in their texture properties in terms of particle sizes, specific surface areas (SSA) and consequently their photocatalytic activity were explained by the role of guanidine hydrochloride in their synthesis. The SSA increased due to the release of NH3 and HCl and its complex reactions with melamine and DCDA forming structure imperfections and disruptions. The photocatalytic activity of the CN materials was found to be dependent on their SSA.
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