Asymmetric structure engineering of polymeric carbon nitride for visible-light-driven reduction reactions

被引:57
作者
Luo, Wei [1 ]
Li, Yongli [1 ]
Wang, Jinshu [1 ]
Liu, Jingchao [1 ]
Zhang, Nan [1 ]
Zhao, Mengdi [1 ]
Wu, Junshu [1 ]
Zhou, Wenyuan [1 ]
Wang, Lianzhou [2 ,3 ]
机构
[1] Beijing Univ Technol, Fac Mat & Manufacture, Key Lab Adv Funct Mat, Beijing 100124, Peoples R China
[2] Univ Queensland, Nanomat Ctr, Sch Chem Engn, St Lucia, Qld 4072, Australia
[3] Univ Queensland, Australian Inst Bioengn & Nanotechnol, St Lucia, Qld 4072, Australia
基金
中国国家自然科学基金;
关键词
Gas-solid grafting reaction; Aromatization; Terminal blocking; Asymmetric structure; Photocatalytic reductions; PHOTOCATALYTIC HYDROGEN; EFFICIENT PHOTOCATALYSTS; EXCITON DISSOCIATION; CHARGE SEPARATION; SOLAR HYDROGEN; NITROGEN; DIOXIDE; G-C3N4; WATER; NANOCOMPOSITES;
D O I
10.1016/j.nanoen.2021.106168
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
The photocatalytic activity of polymeric carbon nitride (g-C3N4) strongly depends on its electronic structure which is highly sensitive to the preparation methods. To design the photocatalysts with efficient charge separation and transfer property, here we report a new ethylenediamine (EDA) induced gas-solid grafting method which enables the asymmetric modification of g-C3N4 featuring the aromatization at the terminal of melon motifs. The obtained terminal-aromatized g-C3N4 (Ar-C3N4) exhibits an improved visible-light-driven photocatalytic activity in versatile two-electron reduction reactions, outperforming the pristine g-C3N4 by 15.4 and 6.6 folds respectively in hydrogen evolution and hydrogen peroxide production. Theoretical and experimental results demonstrate the intensified asymmetry of p-electron distribution in the resulting material, which provides significantly improved driving force to guide the efficient separation of photogenerated e-h pairs and enhance the charge carrier mobility compared to its symmetric counterpart.
引用
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页数:10
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