Tailoring of crystalline structure of carbon nitride for superior photocatalytic hydrogen evolution.

Light absorption and carrier transfer, are two sequential and complementary steps related to photocatalysis performance, whereas the collective integration of these two aspects into graphitic carbon nitride (g-CN) photocatalyst through polycondensation optimization have seldom been achieved. Herein, we report on tailoring the crystalline structure of g-CN by avoiding the formation of incompletely reacted N-rich intermediates and selective breaking the hydrogen bonds between the layers of g-CN simultaneously. The obtained layer plane ordered porous carbon nitride (LOP-CN) material shows efficient photocatalytic H generation performance. The highest H evolution rate achieved is 53.8 μmol under λ ≥ 400 nm light irradiation, which is 7.4 times higher than that of g-CN prepared by convention thermal polycondensation. The substantially boosted photocatalytic activity is mainly ascribed to the efficient charge separation on long-range atomic order layer plane and the extended visible light harvesting ability. This work highlights the importance of crystalline structure tailoring in improving charge separation and light absorption of g-CN photocatalyst for boosting its photocatalytic H evolution activity.