Dopant-Induced Edge and Basal Plane Catalytic Sites on Ultrathin C3N4 Nanosheets for Photocatalytic Water Reduction

被引:79
作者
Zhu, Qiaohong [1 ,2 ]
Qiu, Bocheng [1 ,2 ]
Du, Mengmeng [1 ,2 ]
Ji, Jiahui [1 ,2 ]
Nasir, Muhammad [3 ]
Xing, Mingyang [1 ,2 ]
Zhang, Jinlong [1 ,2 ]
机构
[1] East China Univ Sci & Technol, Sch Chem & Mol Engn, Feringa Nobel Prize Scientist Joint Res Ctr, Key Lab Adv Mat, Shanghai 200237, Peoples R China
[2] East China Univ Sci & Technol, Sch Chem & Mol Engn, Feringa Nobel Prize Scientist Joint Res Ctr, Joint Int Res Lab Precis Chem & Mol Engn, Shanghai 200237, Peoples R China
[3] COMSATS Univ Islamabad, Interdisciplinary Res Ctr Biomed Mat IRCBM, Lahore 54000, Punjab, Pakistan
来源
ACS SUSTAINABLE CHEMISTRY & ENGINEERING | 2020年 / 8卷 / 19期
基金
中国国家自然科学基金;
关键词
dual-doping; catalytic sites; C3N4; hydrogen evolution; photocatalysis; CARBON NITRIDE NANOSHEETS; HYDROGEN EVOLUTION; DOPED G-C3N4;
D O I
10.1021/acssuschemeng.0c02122
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The emerging carbon nitride (C3N4) offers a serious possibility for realizing a highly effective hydrogen evolution reaction (HER). However, their insufficient catalytic sites and poor conductivity hamper the HER performance. Herein, an oxygen, phosphorus dual-doped ultrathin C3N4 nanosheet (O, P-CNS) is synthesized through a two-step method without a liquid solution, including calcination under air and subsequent chemical vapor deposition (CVD) with sodium hypophosphite (NaH2PO2) in N-2 atmosphere. The first thermal treatment in the air atmosphere results in the introduction of O dopant on the edge of C3N4 and the exfoliation of bulk C3N4 into ultrathin nanosheets. The following P incorporation contributes to the activation of the basal plane of C3N4 and the improvement of the intrinsic electronic conductivity, thus giving rise to the facilitated H-2 generation rate. Particularly, a superior H-2 generation rate of 8.7 mmol g(-1) h(-1) under visible light and an apparent quantum yield of 23.65% with 420 nm could be realized after the two-step dual-doping-induced calcination, further confirming the enhanced charge separation with the full activation of the edge and basal plane catalytic sites of C3N4. Our work on dual-doping-induced catalytic site activation on the edge and basal plane of C3N4 will provide more guidance in the field of designing C3N4-based photocatalysts.
引用
收藏
页码:7497 / 7502
页数:6
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