Optimizing the Photocatalytic Hydrogen Evolution Performance of Graphitic Carbon Nitride by Crystallinity Regulation
ZHAO Zhengliang1, SONG Zhenzhen2,3, SHU Zhu4,5,*, ZHOU Jun4,5
1 College of Chemistry and Materials, Taiyuan Normal University, Jinzhong 030619, Shanxi, China 2 Institute of Geographical Science, Taiyuan Normal University, Jinzhong 030619, Shanxi, China 3 Shanxi Key Laboratory of Surface Processes and Resource Ecological Security in Fenhe River Basin, Taiyuan Normal University, Taiyuan 030619, China 4 MOE Engineering Research Center of Nano-Geomaterials, Faculty of Materials Science and Chemistry, China University of Geosciences, Wuhan 430074, China 5 Hubei Three Gorges Laboratory, Yichang 443007, Hubei, China
Abstract: Graphitic carbon nitride (g-C3N4) is a green and safe non-metallic photocatalyst. However, its photocatalytic activity is limited by the low efficiency of photo-generated carrier separation and transfer, while enhancing crystallinity can significantly improve the photocatalytic activity of carbon nitride. Therefore, in this study, a one-step calcination method was employed, using melamine as the precursor and regulating the molar ratios of NH4Cl and NaOH, to successfully synthesize sodium-doped crystalline carbon nitride (NaCCNx, where x refers to the molar ratio of NH4Cl to NaOH), achieving controllable modulation of both in-plane and interlayer crystallinity. Systematic material characterizations revealed that the crystallinity of NaCCNx was significantly enhanced, with NaCCN2.5 exhibiting the optimal in-plane and interlayer crystallinity, along with a substantial improvement in visible light absorption and charge carrier separation and transport efficiency. Under visible-light irradiation, NaCCN2.5 exhibited a superior photocatalytic hydrogen production rate of 1 848 μmol·g-1·h-1, which is 11.6-fold as high as that of bulk g-C3N4. This breakthrough not only confirms the crucial role of crystallinity regulation in enhancing photocatalytic performance, but also provides new ideas and experimental basis for designing efficient non-metallic photocatalysts.
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2026, Vol. 40 
