<p>As one of the most promising metal-free photocatalysts for renewable H<sub>2</sub> evolution, graphitic carbon nitride (g-C<sub>3</sub>N<sub>4</sub>) has attracted notable attention. Regulating its morphology and electronic structure is crucial for enhancing its performance. In this work, aromatic small molecules and melamine were hydrothermally cotreated to form a novel supramolecular precursor, which was subsequently calcined to obtain a π–π conjugated structure of g-C<sub>3</sub>N<sub>4</sub> photocatalyst. The introduction of benzene-ring structures expanded the conjugated system and promoted the excitation of π electrons, thereby broadening the light-absorption range of g-C<sub>3</sub>N<sub>4</sub>. The synergism of bromine and chlorine provided abundant active sites for g-C<sub>3</sub>N<sub>4</sub>, greatly promoted the migration of photogenerated charge carriers, and reduced the recombination probability, thus improving in photocatalytic performance. Therefore, the g-C<sub>3</sub>N<sub>4</sub> photocatalyst obtained from 2-bromo-5-chlorobenzoic acid-derived supramolecular precursor exhibited a visible-light (<i>λ</i> ≥ 400&#xa0;nm) photocatalytic H<sub>2</sub> evolution activity of 839.8&#xa0;μmol/(h&#xa0;g), which was about three times that of the unmodified g-C<sub>3</sub>N<sub>4</sub>. This work offers a novel perspective for g-C<sub>3</sub>N<sub>4</sub> application in the field of photocatalysis and expands the utilization of aromatic small molecules in photocatalysts modification.</p>

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Aromatic Ring-Coordinated g-C3N4 Nanotubes for Enhanced Photocatalytic H2 Evolution

  • Chongze Cai,
  • Huaiyu Lu,
  • Cheng Cheng,
  • Wengao Zeng,
  • Xiangjiu Guan,
  • Liuhao Mao,
  • Li Tian,
  • Jinwen Shi,
  • Liejin Guo

摘要

As one of the most promising metal-free photocatalysts for renewable H2 evolution, graphitic carbon nitride (g-C3N4) has attracted notable attention. Regulating its morphology and electronic structure is crucial for enhancing its performance. In this work, aromatic small molecules and melamine were hydrothermally cotreated to form a novel supramolecular precursor, which was subsequently calcined to obtain a π–π conjugated structure of g-C3N4 photocatalyst. The introduction of benzene-ring structures expanded the conjugated system and promoted the excitation of π electrons, thereby broadening the light-absorption range of g-C3N4. The synergism of bromine and chlorine provided abundant active sites for g-C3N4, greatly promoted the migration of photogenerated charge carriers, and reduced the recombination probability, thus improving in photocatalytic performance. Therefore, the g-C3N4 photocatalyst obtained from 2-bromo-5-chlorobenzoic acid-derived supramolecular precursor exhibited a visible-light (λ ≥ 400 nm) photocatalytic H2 evolution activity of 839.8 μmol/(h g), which was about three times that of the unmodified g-C3N4. This work offers a novel perspective for g-C3N4 application in the field of photocatalysis and expands the utilization of aromatic small molecules in photocatalysts modification.