Citation: Zhangjie Gu, Zhen Shan, Yulan Wang, Jinjian Wang, Tongtong Liu, Xiaoming Li, Zhiyang Yu, Jian Su, Gen Zhang. Tuning the exciton binding energy of covalent organic frameworks for efficient photocatalysis[J]. Chinese Chemical Letters, ;2024, 35(2): 108356. doi: 10.1016/j.cclet.2023.108356 shu

Tuning the exciton binding energy of covalent organic frameworks for efficient photocatalysis

Zhangjie Gu ^a ,
Zhen Shan ^a ,
Yulan Wang ^b ,
Jinjian Wang ^a ,
Tongtong Liu ^a ,
Xiaoming Li ^c ,
Zhiyang Yu ^b ,
Jian Su ^{a, *,} ,
Gen Zhang ^{a, d, *,}

a.
Key Laboratory for Soft Chemistry and Functional Materials of Ministry of Education, School of Chemistry and Chemical Engineering, Nanjing University of Science and Technology, Nanjing 210094, China
b.
State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou 350002, China
c.
MIIT Key Laboratory of Advanced Display Material and Devices, School of Materials Science and Engineering, Nanjing University of Science and Technology, Nanjing 210094, China
d.
Key Laboratory of Preclinical Study for New Drugs of Gansu Province, School of Basic Medical Sciences, Lanzhou University, Lanzhou 730000, China

sujian@njust.edu.cn

zhanggen@njust.edu.cn

Received Date: 31 January 2023
Revised Date: 19 February 2023
Accepted Date: 20 March 2023
Available Online: 22 March 2023

Figures(6)

Owing to the large exciton binding energy (>100 meV) of most organic materials, the process of exciton dissociation into free electrons and holes is seriously hindered, which plays a key role in the photocatalytic system. In this study, a series of chalcogen (S, Se)-substituted mesoporous covalent organic frameworks (COFs) have been synthesized for enhanced photocatalytic organic transformations. Photoelectrochemical measurements indicate that the introduction of semi-metallic Se atom and the enlargement of conjugation degree can not only reduce the exciton binding energy accelerating the charge separation, but also reduce the band gap of COFs. As a result, the COF-NUST-36 with the lowest exciton binding energy (39.5 meV) shows the highest photocatalytic performance for selective oxidation of amines (up to 98% Conv. and 97.5% Sel.). This work provides a feasible method for designing COFs with high photocatalytic activity by adjusting exciton binding energy.
- Covalent organic frameworks,
- Exciton binding energy,
- Atom substitution,
- Extended conjugation,
- Photocatalysis
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