Tuning Heptazine-Based g‑C₃N₄ Structures for Photocatalysis by Enhancing Chemical Stability and Electron-Hole Pair...

Area of Science:

• Materials Science
• Photocatalysis
• Computational Chemistry

Background:

• Graphitic carbon nitride (g-C3N4) is a promising photocatalyst due to its charge-transfer properties and tunable band structure.
• Current limitations include low visible-light absorption and rapid electron-hole pair recombination, hindering photocatalytic efficiency.

Purpose of the Study:

• To computationally investigate the effects of Boron (BH) and Hydrogen (NH) substitution on g-C3N4 building blocks.
• To explore strategies for enhancing charge transfer and visible-light absorption in g-C3N4 photocatalysts.

Main Methods:

• Density Functional Theory (DFT) calculations were employed.
• Investigated the influence of BH and NH substitutions on g-C3N4 properties.
• Analyzed the energetic alignment with Standard Hydrogen Electrode (SHE) and Oxygen Evolution Reaction (OER) potentials.

Main Results:

• BH substitution creates electron-deficient regions, promoting charge transfer and enhancing photocatalytic activity.
• NH substitution adjusts excitation energy levels, shifting absorption into the visible spectrum and optimizing alignment with SHE and OER potentials.
• Combining BH and NH substitutions in a single model enhances light absorption and reduces electron-hole recombination without compromising individual properties.

Conclusions:

• BH and NH substitutions offer a viable strategy to improve g-C3N4 photocatalyst performance.
• Combining these substitutions presents a promising approach for developing efficient visible-light-driven photocatalysts.
• The findings highlight the potential for synergistic effects in engineered photocatalytic materials.