Three-Component Donor-?-Acceptor Covalent-Organic Frameworks for Boosting Photocatalytic Hydrogen Evolution

Li, Ziping1; Deng, Tianqi2,3; Ma, Si1; Zhang, Zhenwei1; Wu, Gang2; Wang, Jiaao4,5; Li, Qizhen6; Xia, Hong7; Yang, Shuo-Wang2; Liu, Xiaoming1

2023-03-01

10.1021/jacs.2c11893

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY   影响因子和分区

0002-7863

1520-5126

Two-dimensional covalent-organic frameworks (2D COFs) have recently emerged as great prospects for their applications as new photocatalytic platforms in solar to-hydrogen conversion; nevertheless, their inefficient solar energy capture and fast charge recombination hinder the improvement of photocatalytic hydrogen production performance. Herein, two photoactive three-component donor-pi-acceptor (TCDA) materials were constructed using a multicomponent synthesis strategy by introducing electron deficient triazine and electron-rich benzotrithiophene moieties into frameworks through sp2 carbon and imine linkages, respectively. Compared with two-component COFs, the novel TCDA-COFs are more convenient in regulating the inherent photophysical properties, thereby realizing outstanding photocatalytic activity for hydrogen evolution from water. Remarkably, the first sp2 carbon-linked TCDA-COF displays an impressive hydrogen evolution rate of 70.8 +/- 1.9 mmol g-1 h-1 with excellent reusability in the presence of 1 wt % Pt under visible-light illumination (420-780 nm). Utilizing the combination of diversified spectroscopy and theoretical prediction, we show that the full pi-conjugated linkage not only effectively broadens the visible-light harvesting of COFs but also enhances charge transfer and separation efficiency.

SCI

英语

NI论文 ; ESI热点 ; ESI高被引

其他

National Science Foundation of China["52073119","62075081","21774040"]

Chemistry

Chemistry, Multidisciplinary

WOS:000950912900001

AMER CHEMICAL SOC

Web of Science

1.Jilin Univ, Coll Chem, Changchun 130012, Peoples R China
2.Agcy Sci Technol & Res, Inst High Performance Comp, Singapore 138632, Singapore
3.Zhejiang Univ, Hangzhou Global Sci & Technol Innovat Ctr, Hangzhou 311200, Peoples R China
4.Univ Texas Austin, Dept Chem, Austin, TX 78712 USA
5.Univ Texas Austin, Oden Inst Computat Engn & Sci, Austin, TX 78712 USA
6.Southern Univ Sci & Technol, Dept Biomed Engn, Shenzhen 518055, Peoples R China
7.Jilin Univ, Coll Elect Sci & Technol, State Key Lab Integrated Optoelect, Changchun 130012, Peoples R China

Li, Ziping,Deng, Tianqi,Ma, Si,et al. Three-Component Donor-?-Acceptor Covalent-Organic Frameworks for Boosting Photocatalytic Hydrogen Evolution[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,2023,145(15).

Li, Ziping.,Deng, Tianqi.,Ma, Si.,Zhang, Zhenwei.,Wu, Gang.,...&Liu, Xiaoming.(2023).Three-Component Donor-?-Acceptor Covalent-Organic Frameworks for Boosting Photocatalytic Hydrogen Evolution.JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,145(15).

Li, Ziping,et al."Three-Component Donor-?-Acceptor Covalent-Organic Frameworks for Boosting Photocatalytic Hydrogen Evolution".JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 145.15(2023).