Oriented transfer of electron-hole charge carriers is important during photocatalytic processes. In this study, one-dimensional (1D) tubular B-doped graphitic carbon nitride (g-C₃N₄) with an effective charge transfer and separation was designed. The doping sites, energy level structure, and photo-generated electron-hole pair separation were predicted using systematical density functional theory (DFT) simulations. The supramolecular precursor for tubular g-C₃N₄ synthesis, namely melamine·cyanuric acid (M·CA), was controllably synthesized from a single melamine source. Intermolecular hydrogen bonding led to the arrangement of supramolecular aggregate structures into a prismatic crystal architecture during the hydrothermal treatment. The morphology modulation of g-C₃N₄ from bulk to 1D tubular architecture was realized by calcining the prism-like precursor. B-doped tubular g-C₃N₄ exhibited a narrower band-gap, multiple reflections of incident light, and oriented transfer of electron-hole charge carriers, which led to a widened light-harvesting range and improved photo-induced electron-hole pair separation and transfer ability. These factors contributed to the photocatalytic activity enhancement towards gaseous NOx degradation under visible light. In this work, a valuable design-fabrication pattern for g-C₃N₄ modification and engineering via DFT simulations was designed. Moreover, a strategy was developed for the simultaneous foreign atom doping and architecture control of g-C₃N₄ via the self-assembly of supramolecular precursors. Copyright © 2018 Elsevier B.V. All rights reserved.
CitationWang, Z., Chen, M., Huang, Y., Shi, X., Zhang, Y., Huang, T., . . . Lee, S. C. (2018). Self-assembly synthesis of boron-doped graphitic carbon nitride hollow tubes for enhanced photocatalytic NOₓ removal under visible light. Applied Catalysis B: Environmental, 239, 352-361. doi: 10.1016/j.apcatb.2018.08.030
- DFT predictions
- 1D tubular g-C₃N₄
- Photocatalytic NO removal