As an efficient photocatalyst, graphitic carbon nitride (g-C3N4) has been widely used in the field of photocatalytic hydrogen production. However, how to prepare hydrogen efficiently and stably has become a challenge. Herein, we successfully realize metal-free edge modification with phenyl groups by one-step thermal polymerization of urea with 4-phenyl-3-thiosemicarbazide. Consequently, the optimal photocatalytic hydrogen production rate for the modified graphitic carbon nitride is increased by three times to a value of 2390.6 μmol h-1 g-1, while the apparent quantum efficiency (AQE) reaches 8.3 % at a wavelength of 420 nm. We also provide a theoretical explanation for the experiments using density functional theory (DFT) calculations, which suggest that energy level changes and electron redistribution for the modified carbon nitride materials contribute to the observed changes in catalytic performance. This work provides an effective solution for improving the photocatalytic activity of carbon nitride materials and provides theoretical support for the edge modification of carbon nitride materials to promote their photocatalytic hydrogen production efficiency.
Keywords: Band gap regulation; DFT; Effective charge separation; Nonmetal group modification; Photocatalytic hydrogen production; g-C(3)N(4).
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