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

Zhangjie Gu ¹Zhen Shan ¹Yulan Wang ²Jinjian Wang ¹Tongtong Liu ¹Xiaoming Li ³Zhiyang Yu ²Jian Su ¹Gen Zhang⁴

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作者信息

1. 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
2. State Key Laboratory of Photocatalysis on Energy and Environment,College of Chemistry,Fuzhou University,Fuzhou 350002,China
3. MIIT Key Laboratory of Advanced Display Material and Devices,School of Materials Science and Engineering,Nanjing University of Science and Technology,Nanjing 210094,China
4. 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;Key Laboratory of Preclinical Study for New Drugs of Gansu Province,School of Basic Medical Sciences,Lanzhou University,Lanzhou 730000,China
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Abstract

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 photocat-alytic system.In this study,a series of chalcogen(S,Se)-substituted mesoporous covalent organic frame-works(COFs)have been synthesized for enhanced photocatalytic organic transformations.Photoelectro-chemical 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.

Key words

Covalent organic frameworks/Exciton binding energy/Atom substitution/Extended conjugation/Photocatalysis

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基金项目

国家自然科学基金(22171136)

江苏省自然科学基金(BK20220928)

江苏省自然科学基金(BK20220079)

中央高校基本科研业务费专项(30921011102)

中央高校基本科研业务费专项(30922010902)

Medical Innovation and Development Project of Lanzhou University(lzuyxcx-2022-156)

Chinese Academy of Medical Sciences(CAMS)Innovation Fund for Medical Sciences(2019-I2M-5-074)

Chinese Academy of Medical Sciences(CAMS)Innovation Fund for Medical Sciences(2021-I2M-1-026)

Chinese Academy of Medical Sciences(CAMS)Innovation Fund for Medical Sciences(2021-I2M-3-001)

Startup Funding from Nanjing University of Science and Technology(AE89990)

Startup Funding from Nanjing University of Science and Technology(AE89991/376)

Thousand Young Talent Plan()

出版年

2024

中国化学快报(英文版)

中国化学会

中国化学快报(英文版)

CSTPCD

影响因子：0.771

ISSN：1001-8417

参考文献量59

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