In this work, two new N-annulated perylene-based organic sensitizers (PY-1 and PY-2) have been developed for dye-sensitized graphitic carbon nitride (g-C₃N₄) to remarkably enhance photocatalytic hydrogen production under visible-light irradiation (420 nm ≤ λ ≤ 780 nm). The results showed that the H₂ production rates of the PY-1/g-C₃N₄/Pt and PY-2/g-C₃N₄/Pt were up to 5508.1 μmol h⁻¹ g⁻¹ and 11,855.4 μmol h⁻¹ g⁻¹, respectively, which were 8.98 and 19.3 times higher than that of the g-C₃N₄/Pt, respectively. Specifically, an impressive record apparent quantum efficiency (AQY) of 27.16% for PY-2/g-C₃N₄/Pt system was achieved at λ = 550 nm monochromatic light irradiation. Moreover, the formation of amide bonds between dye molecules and g-C₃N₄ was firstly confirmed by FTIR spectrum and theoretical calculation. The amide bonds provided the electron transfer channels to significantly improve interface charge transfer and separation, thus resulting in a more efficient hydrogen production. More importantly, PY-1/g-C₃N₄/Pt and PY-2/g-C₃N₄/Pt displayed good stability under long-term irradiation and was favorable and significant for practical application. Our work indicated that dye sensitized g-C₃N₄ to form an amide bond is a promising strategy to realize the effective conversion of solar energy to hydrogen energy through molecular engineering.

在这项工作中，已开发出两种新型的N环per基有机增感剂（PY-1和PY-2）用于染料敏化的石墨碳氮化物（gC ₃ N ₄），以显着提高可见光照射下的光催化产氢量。 （420 nm≤λ≤780 nm）。结果表明，PY-1 / gC ₃ N ₄ / Pt和PY-2 / gC ₃ N ₄ / Pt的H ₂生产率分别达到5508.1μmolh ^-1 g ^-1和11,855.4μmolh ^-1 g ^-1分别比gC ₃ N ₄ / Pt高8.98倍和19.3倍。具体而言，在λ= 550 nm单色光照射下，PY-2 / gC ₃ N ₄ / Pt体系的表观量子效率（AQY）达到了令人印象深刻的27.16％。此外，首先通过FTIR光谱和理论计算证实了染料分子与gC ₃ N ₄之间的酰胺键的形成。酰胺键提供了电子转移通道，可显着改善界面电荷的转移和分离，从而提高了产氢效率。更重要的是，PY-1 / gC ₃ N₄ / Pt和PY-2 / gC ₃ N ₄ / Pt在长期辐照下显示出良好的稳定性，对实际应用具有良好的意义。我们的工作表明，染料敏化的gC ₃ N ₄形成酰胺键是一种通过分子工程实现将太阳能有效转化为氢能的有前途的策略。