General surface grafting strategy-derived carbon-modified graphitic carbon nitride with largely enhanced visible light photocatalytic H2 evolution coupled with benzyl alcohol oxidation

被引:36
作者
Wang, Haifei [1 ]
Zhang, Jihua [3 ]
Jin, Xu [2 ]
Wang, Xiaoqi [2 ]
Zhang, Fu [1 ]
Xue, Jierui [1 ]
Li, Yapeng [1 ]
Li, Jianming [2 ]
Zhang, Genqiang [1 ]
机构
[1] Univ Sci & Technol China, Dept Mat Sci & Engn, CAS Key Lab Mat Energy Convers, Hefei Natl Lab Phys Sci Microscale, Hefei 230026, Anhui, Peoples R China
[2] PetroChina, Res Inst Petr Explorat & Dev RIPED, Beijing 100083, Peoples R China
[3] Guizhou Educ Univ, Guizhou Prov Key Lab Computat Nanomat Sci, Guiyang 550018, Guizhou, Peoples R China
基金
中国国家自然科学基金;
关键词
HYDROGEN EVOLUTION; QUANTUM DOTS; GRAPHENE; WATER; NANOSHEETS; G-C3N4; SEMICONDUCTORS; COMPOSITES; POLYMERS;
D O I
10.1039/d1ta00142f
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Carbon-modified g-C3N4 manifests increasing prospects in the photocatalytic realm. However, there are some challenges, such as difficult large-scale preparation, weak interface connection, limited active sites, and inefficient light utilization, which restrain the further utilization for carbon modified g-C3N4. To solve these disadvantages, we recommended a novel and general surface grafting strategy followed by the in situ carbonization treatment to obtain carbon-modified graphitic carbon nitride (CMCN). Experimental results disclose that the introduced carbon connected intimately with g-C3N4 by edge N atoms, which dramatically improve the charge transfer kinetics. CMCN presents incredibly reinforced visible light photocatalytic activity with an impressive hydrogen evolution rate of 5.549 mmol g(-1) h(-1), which is about 13.3 times higher than that of pure g-C3N4. Theoretical calculation results show that the introduced carbon can form a new intermediate state between the bandgap, which could capture the photoexcited electrons and reinforce the visible light absorption. Importantly, the practicality of the CMCN material is further demonstrated by replacing a sacrificial reagent with benzyl alcohol conversion to produce value-added benzaldehyde, where the decent evolution rates of 0.288 and 0.230 mmol g(-1) h(-1) can be achieved for H-2 and benzaldehyde, respectively.
引用
收藏
页码:7143 / 7149
页数:7
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