Synergy of defect engineering and curvature effect for porous graphite carbon nitride nanotubes promoted photocatalytic hydrogen evolution

EcoEnergy Pub Date : 2023-12-21 DOI:10.1002/ece2.20
Liping Guo, Jinyu Gao, Mingxia Li, Ying Xie, Hui Chen, Shijie Wang, Zhenzi Li, Xuepeng Wang, Wei Zhou
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Abstract

Graphite carbon nitride (g-C3N4) nanotubes have received extensive attention due to its unique morphology and electronic migration. Herein, the defective porous g-C3N4 nanotube (DTCN) is prepared through a simple thermal reduction process. The construction of N vacancy and tubular structure can synergistically promote the separation of photogenerated charge carriers. As a result, DTCN demonstrates a higher photocatalytic hydrogen evolution rate (1440 μmol·g−1·h−1), which is 5 times higher than that of the initial g-C3N4 nanotube (TCN). Importantly, combined with density functional theory calculations and experimental results, it is the first time to prove that the synergy of curvature effect and N vacancy of nanotubes can enhance the adsorption energy of hydrogen and decrease the work function, resulting in more superior photocatalytic performance than the layered structure. This work provides more in-depth comprehension for the photocatalytic mechanism of nanotube materials, which has inspirational significance for the design of the g-C3N4 photocatalyst with high performance.

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多孔石墨氮化碳纳米管缺陷工程与曲率效应的协同作用促进光催化氢进化
氮化石墨碳(g-C3N4)纳米管因其独特的形态和电子迁移而受到广泛关注。本文通过简单的热还原工艺制备了缺陷多孔 g-C3N4 纳米管(DTCN)。N 空位和管状结构的构建能协同促进光生电荷载流子的分离。因此,DTCN 具有更高的光催化氢进化率(1440 μmol-g-1-h-1),是初始 g-C3N4 纳米管(TCN)的 5 倍。重要的是,结合密度泛函理论计算和实验结果,首次证明了纳米管的曲率效应和 N 空位的协同作用可以提高氢的吸附能并降低功函数,从而获得比层状结构更优越的光催化性能。该研究对纳米管材料的光催化机理有了更深入的理解,对高性能 g-C3N4 光催化剂的设计具有启发意义。
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