Metal-Oxide-Mediated Subtractive Manufacturing of Two-Dimensional Carbon Nitride for High-Efficiency and High-Yield Photocatalytic H2 Evolution

被引:139
作者
Xu, Hui [1 ]
She, Xiaojie [1 ]
Fei, Ting [1 ]
Song, Yanhua [2 ]
Liu, Daobin [3 ]
Li, Hongping [1 ]
Yang, Xiaofei [4 ]
Yang, Jinman [1 ]
Li, Huaming [1 ]
Song, Li [3 ]
Ajayan, Pulickel M. [5 ]
Wu, Jingjie [6 ]
机构
[1] Jiangsu Univ, Sch Environm & Safety Engn, Inst Energy Res, Zhenjiang 212013, Jiangsu, Peoples R China
[2] Jiangsu Univ Sci & Technol, Sch Environm & Chem Engn, Zhenjiang 212003, Jiangsu, Peoples R China
[3] Univ Sci & Technol China, Natl Synchrotron Radiat Lab, Hefei 230029, Anhui, Peoples R China
[4] Nanjing Forestry Univ, Inst Mat Phys & Chem, Sch Sci, Nanjing 210037, Jiangsu, Peoples R China
[5] Rice Univ, Dept Mat Sci & NanoEngn, Houston, TX 77005 USA
[6] Univ Cincinnati, Dept Chem & Environm Engn, Cincinnati, OH 45221 USA
基金
中国博士后科学基金; 中国国家自然科学基金;
关键词
two-dimensional carbon nitride; catalytic synthesis; 2D/2D composites; Z-scheme heterojunction; photocatalytic hydrogen evolution; GAS SHIFT REACTION; HYDROGEN-PRODUCTION; CHARGE-TRANSFER; QUANTUM DOTS; NANOSHEETS; WATER; MECHANISM; ABSORPTION; GRAPHENE;
D O I
10.1021/acsnano.9b04443
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
g-C3N4 is a promising visible-light-driven photo-catalyst for H-2 evolution reaction; however, the achievement of the high photocatalytic performance is primarily limited by the low separation efficiency of the photogenerated charge carriers and partly restricted by the slow kinetics of charge transfer. 2D g-C(3)N(4 )can significantly improve the charge generation, transfer, and separation efficiencies. The 2D g-C3N4-based Z-scheme heterostructure can further enhance the charge-carrier separation and simultaneously increase the redox ability, thereby further boosting the photocatalytic performance. Here we report a transition-metal-oxide (TMO)-mediated subtractive manufacturing process toward the large-scale synthesis of 2D g-C3N4 and the simultaneous formation of a 2D/2D TMO/g-C3N4 Z-scheme heterojunction. The TMOs serve as catalysts to facilitate the hydrolysis reaction of the bulk g-C3N4 in the presence of moist air, forming 2D g-C3N4. The resulting 2D/2D TMO/g-C3N4 catalysts, in particular, 2D/2D Co3O4/g-C3N4, exhibit high-efficiency and high-yield photocatalytic H-2 evolution due to the suppression of electron-hole pair recombination and enhanced redox ability. The 2D/2D Co3O4/g-C3N4 photocatalyzes the H-2 evolution with a rate of, similar to 370 mu mol h(-1) within lambda > 400 nm. The external quantum efficiency of 2D/2D Co3O4/g-C3N4 at lambda = 405 nm reaches 53.6%, which is among the highest values for g-C3N4-based catalysts.
引用
收藏
页码:11294 / 11302
页数:9
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