Controlled synthesis of hollow carbon ring incorporated g-C3N4 tubes for boosting photocatalytic H2O2 production

被引:56
|
作者
Luo, Hao [1 ]
Shan, Tianshang [1 ]
Zhou, Jianwen [1 ]
Huang, Liulian [1 ]
Chen, Lihui [1 ]
Sa, Rongjian [2 ]
Yamauchi, Yusuke [3 ,4 ,5 ,6 ]
You, Jungmok
Asakura, Yusuke [3 ]
Yuan, Zhanhui [1 ]
Xiao, He [1 ]
机构
[1] Fujian Agr & Forestry Univ, Coll Mat Engn, Fuzhou 350108, Fujian, Peoples R China
[2] Minjiang Univ, Coll Mat & Chem Engn, Fuzhou 350108, Peoples R China
[3] Nagoya Univ, Grad Sch Engn, Dept Mat Proc Engn, Furo Cho,Chikusa Ku, Nagoya 4648603, Japan
[4] Univ Queensland, Sch Chem Engn, Brisbane, Qld 4072, Australia
[5] Univ Queensland, Australian Inst Bioengn & Nanotechnol AIBN, Brisbane, Qld 4072, Australia
[6] Kyung Hee Univ, Coll Life Sci, Dept Plant & Environm New Resources, 1732 Deogyeong Daero, Yongin 17104, Gyeonggi Do, South Korea
基金
中国博士后科学基金;
关键词
Carbon nitride; Photocatalytic; Hydrogen peroxide; Carbon rings; HYDROGEN-PEROXIDE; OXYGEN REDUCTION; NITRIDE; NANOSHEETS; WATER; EVOLUTION; NANOSTRUCTURES; SEPARATION; NANOTUBES; DEFECTS;
D O I
10.1016/j.apcatb.2023.122933
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
H2O2 production through solar-driven photocatalytic route has received increasing attention. Herein, a carbon ring incorporated hollow g-C3N4 tubes (CHCN) was successfully fabricated via a novel supramolecular selfassembly strategy, co-inducing by hydrogen bond and covalent bond. The optimum H2O2 yield over the CHCN-0.02 reached up to 1.58 mmol L-1 h-1 (AQE= 28.10%, 420 nm), which was 5.4 times significantly higher than that of bulk g-C3N4 (0.29 mmol L-1 h-1) under visible light irradiation. Experimental and density functional theory (DFT) calculations revealed that the CHCNs not only expedited the charge carrier transfer/separation but also favored molecular oxygen adsorption and regulated bandgap structure under the in-plane electronic field induced by continuous & pi;-conjugated Cring, which boosted the ORR efficiency for photocatalytic H2O2 synthesis. The optimized CHCN catalyst demonstrated adequate hybrid ORR routes, consisting of a dominated selective one-step two-electron ORR pathway and highly efficient two-step single-electron ORR for H2O2 production. Therefore, this work not only provides a new strategy for an efficient H2O2 formation using a g-C3N4-based photocatalyst but also explores the functionary mechanism of the ORR process and enlightens the way to highly efficient H2O2 generation.
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页数:13
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