4.7 Article

Surface oxygenous groups modified graphitic carbon nitride with significant positive shift of valence band for efficient photocatalytic oxidation

Journal

APPLIED SURFACE SCIENCE
Volume 563, Issue -, Pages -

Publisher

ELSEVIER
DOI: 10.1016/j.apsusc.2021.150070

Keywords

g-C3N4; Functional group; Oxidation ability; Photogenerated holes; Photocatalysis

Funding

  1. Guangdong Provincial Key Laboratory of Energy Materials for Electric Power [2018B030322001]
  2. Guangdong Provincial Key Laboratory of Catalysis [2020B121201002]
  3. Shenzhen Clean Energy Research Institute [CERI-KY-2019-003]
  4. Shenzhen Key Laboratory of Solid State Batteries [ZDSYS20180208184346531]
  5. National Natural Science Foundation of China [21703097]
  6. Postdoctoral Research Foundation of China [2017M611446]
  7. Development and Reform Commission of Shenzhen Municipality

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Refluxing g-C3N4 in H2O2 introduces oxygenous groups into the material, significantly improving its hydrophilic ability and photocatalytic oxidative ability. The positive shift in valence band position due to the introduction of surface oxygenous groups enhances the photocatalytic activity. Further improvement in photocatalytic oxidative activity can be achieved by forming g-C3N4/TiO2 nanocomposites during the H2O2 reflux treatment, leading to increased driving force and accelerated charge migration.
Graphitic carbon nitride (g-C3N4) is a remarkable metal-free photocatalyst which is widely used for photocatalytic reductive reaction due to its suitable potential of conduction band, but also suffers from intrinsically weak photocatalytic oxidation ability. Here, by simply refluxing g-C3N4 in H2O2, oxygenous groups are introduced into g-C3N4. The resultant oxygenous groups modified g-C3N4 (g-C3N4 (H2O2)) exhibits significantly improved hydrophilic ability and photocatalytic oxidative ability. It is well evidenced that valence band position is positive shifted significantly by introduction of surface oxygenous groups. However, the photocatalytic activity for oxygen evolution is not improved obviously, suggesting that the driving force for water oxidation is not increased simultaneously. Luckily, the photocatalytic oxidative activity of the modified g-C3N4 (include oxygen evolution, pollutant degradation and antibacterial property) could be further improved after forming TiO2 containing nanocomposites during the H2O2 reflux treatment with the addition of tertrabutyl titanate (g-C3N4/ TiO2 (H2O2) due to much increased driving force and accelerated charge migration. Herein, a facile and simple method is proposed to engineer the band structure of g-C3N4 for improving its photocatalytic oxidative ability, which expand the application of carbon nitride.

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