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Precursor-Engineering Coupled Microwave Molten-Salt Strategy Enhances Photocatalytic Hydrogen Evolution Performance of g-C3N4 Nanostructures

Journal 2019 · IF 7.804 · 13(4): 827-837 · 发表于 2019 年 11 月 29 日
作者: Huijuan Jing,Mingzhu You,Shasha Yi,Tao Li,Haipeng Ji,Yu Wang,Zongtao Zhang,Rui Zhang,Deliang Chen,Huaming Yang
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摘要

Graphical Precursors and blessings : A precursor-engineering strategy coupled with a microwave molten-salt process is developed to synthesize g-C 3 N 4 with an isotype triazine/heptazine-based g-C 3 N 4 heterojunction as a photocatalyst for the hydrogen evolution reaction (HER) under visible light illumination. The promising HER activity is attributed to the composition and microstructure, efficient separation of electron–hole pairs, broadened photo-absorption edges, and narrowed band gaps. A precursor-engineering strategy coupled with a microwave molten-salt process (PE-MWMS) is developed to synthesize graphitic carbon nitride (g-C 3 N 4 ) with an isotype triazine/heptazine-based g-C 3 N 4 heterojunction as a photocatalyst for the hydrogen evolution reaction (HER) under visible light illumination. Four hybrid precursor combinations—thiourea/melamine, thiourea/dicyandiamide, urea/melamine, and urea/dicyandiamide—are used to synthesize g-C 3 N 4 heterojunctions by the PE-MWMS process. Control experiments indicate that the precursor components and microwave treatment have a great effect on the HER performance of the g-C 3 N 4 samples. Samples synthesized with the optimal molar ratios of thiourea/melamine (2:1), thiourea/dicyandiamide (2:1), urea/melamine (3:1), and urea/dicyandiamide (3:1), exhibit the highest HER rates of 3135, 2519, 2844, and 2565 μmol g −1 h −1 , respectively. The amounts of heptazine and triazine units in the g-C 3 N 4 samples can be easily adjusted by changing the ratios of the hybrid precursors and play a decisive role in improving the photocatalytic HER activity. Because of the unique composition and microstructure, the efficient separation of electron–hole pairs, the broadened photo-absorption edges, and the narrowed band gaps, the as-obtained triazine/heptazine-based g-C 3 N 4 nanostructures exhibit promising activity for HER application.