期刊
APPLIED CATALYSIS B-ENVIRONMENTAL
卷 280, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.apcatb.2020.119461
关键词
Nanoconfined synthesis; Vertical graphene; Plasma nanofabrication; Edge effect; Hydrogen evolution
资金
- National Natural Science Foundation of China [51722604, 52061130218]
- Zhejiang Provincial Natural Science Foundation of China [LR17E060002]
- Australian Research Council
- QUT Centre for Materials Science
- State Key Laboratory of Clean Energy Utilization Open Fund [ZJUCEU2019002]
In this study, a rational design of confined synthesis of g-C3N4 nanomeshes on N-doped vertically-oriented graphene arrays was reported for enhanced hydrogen evolution. The well-defined hierarchical architecture of the GCN/NVG photocatalyst not only effectively avoided aggregation of 2D g-C3N4 nanosheets, but also demonstrated superaerophobicity and enhanced light absorption. Experimental and simulation results suggest that the protruding graphene edges induce charge redistribution, leading to enhanced interfacial charge separation and high hydrogen evolution rates in water and simulated seawater.
Two-dimensional photocatalysts often suffer severe aggregation due to the inevitable van der Waals forces between nanosheets, which limits their photocatalytic water-splitting efficiency. Herein, a rational design of confined synthesis of g-C3N4 nanomeshes (GCN) on N-doped vertically-oriented graphene (NVG) arrays for enhanced hydrogen evolution is reported. The aggregation of 2D g-C3N4 nanosheets is effectively avoided via physical separation by electrically conductive NVG networks. Well-defined hierarchical architecture of the GCN/NVG photocatalyst endows with superaerophobicity and simultaneously enhanced light absorption. Experimental and ab initio simulation results suggest that the protruding graphene edges induce charge redistribution, thus enhancing interfacial charge separation. The GCN/NVG samples demonstrate a high areal hydrogen evolution rate of 41.7 mu mol h(-1) cm(-2) (225L m(-2) in 24h, STP) in water and 45.8 mu mol h(-1) cm(-2) (246.2 L m(-2) in 24 h, STP) in simulated seawater. This work creates further opportunities for the development of earth-abundant photocatalysts.
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