What does graphitic carbon nitride really look like?

文献情報

出版日 2021-01-11

DOI 10.1039/D0CP06063A

インパクトファクター 3.676

著者

Sigismund T. A. G. Melissen, Tangui Le Bahers, Stephan N. Steinmann

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要旨

Graphitic carbon nitrides (g-CNs) have become popular light absorbers in photocatalytic water splitting cells. Early theoretical work on these structures focused on fully polymerized g-C3N4. Experimentally, it is known that the typically employed melamine polycondensation does not go toward completion, yielding structures with ∼15 at% hydrogen. Here, we study the conformational stability of “melon”, with the [C6N9H3]n structural formula using DFT. Referencing to a 2D melon sheet, B3LYP-dDsC and PBE-MBD computations revealed the same qualitative trend in stability of the 3D structures, with several of them within 5 kJ mol−1 per tecton. Fina's orthorhombic melon is the most stable of the studied conformers, with Lotsch' monoclinic melon taking an intermediate value. Invoking a simple Wannier–Mott-type approach, Fina's and Lotsch' structures exhibited the lowest optical gaps (2.8 eV), within the error margin of the experimental value (2.7 eV). All conformers yielded gaps below that of the monolayer's (3.2 eV), suggesting Jelley-type (“J”) aggregation effects.

掲載誌

Physical Chemistry Chemical Physics

CiteScore: 5.5

自己引用率: 10.3%

年間論文数: 3036

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