Enhanced CO2 Photoreduction through Spontaneous Charge Separation in End-Capping Assembly of Heterostructured Covalent-Organic Frameworks
2022-11
发表期刊ANGEWANDTE CHEMIE - INTERNATIONAL EDITION (IF:16.1[JCR-2023],16.2[5-Year])
ISSN1433-7851
EISSN1521-3773
卷号61期号:50
发表状态已发表
DOI10.1002/anie.202214142
摘要

It is well known that charge separation is crucial for efficient photocatalytic solar conversion. Although some covalent-organic frameworks (COFs) exhibit visible-light harvest, the large exciton binding energies reduce their photocatalytic efficiencies. Herein, we developed a novel method to post-treat the olefin-linked COFs with end-capping polycyclic aromatic hydrocarbons (PAHs) for spontaneous charge separation. Interestingly, a type-II heterostructure is constructed in our perylene-modified COFs which displays drastically enhanced performance for photocatalytic CO2 reduction, with an efficiency of 8-fold higher than that of unmodified COF. A combination of electrochemical, steady-state, and time-resolved spectroscopic measurements indicates that such drastically enhanced performance should be attributed to photoinduced spontaneous charge separation in the heterostructure. These results illustrate the feasibility of engineering the charge-separation properties of crystalline porous frameworks at a molecular level for artificial photosynthesis. © 2022 Wiley-VCH GmbH.

关键词Artificial photosynthesis Binding energy Carbon dioxide Efficiency Electron transitions Photocatalytic activity Reduction Separation Charge-separation CO 2 reduction Covalent organic frameworks End capping Exciton-binding energy Performance Photo reduction Photo-catalytic Postsynthetic modification Visible light
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收录类别SCI ; SCIE ; EI
语种英语
资助项目National Natural Science Foundation of China[
WOS研究方向Chemistry
WOS类目Chemistry, Multidisciplinary
WOS记录号WOS:000880976600001
出版者John Wiley and Sons Inc
EI入藏号20224613110204
EI主题词Polycyclic aromatic hydrocarbons
EI分类号657.1 Solar Energy and Phenomena ; 801.4 Physical Chemistry ; 802.2 Chemical Reactions ; 802.3 Chemical Operations ; 804.1 Organic Compounds ; 804.2 Inorganic Compounds ; 913.1 Production Engineering
原始文献类型Article in Press
Scopus 记录号2-s2.0-85141714717
来源库Scopus
引用统计
被引频次:92[WOS]   [WOS记录]     [WOS相关记录]
文献类型期刊论文
条目标识符https://kms.shanghaitech.edu.cn/handle/2MSLDSTB/248920
专题物质科学与技术学院
物质科学与技术学院_博士生
作者单位
1.State Key Laboratory of Structural Chemistry,Fujian Institute of Research on the Structure of Matter,Chinese Academy of Sciences,Fuzhou,Fujian,350108,China
2.State Key Laboratory of Molecular Reaction Dynamics,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian,Liaoning,116023,China
3.School of Physical Science and Technology,ShanghaiTech University,Shanghai,201210,China
4.Jiangxi Key Laboratory of Organic-Pharmaceutical Chemistry,College of Chemistry and Chemical Engineering,Gannan Normal University,Ganzhou,Jiangxi,341000,China
5.College of Geography and Environmental Engineering,Gannan Normal University,Ganzhou,Jiangxi,341000,China
6.School of Chemical Engineering and Light Industry,Guangdong University of Technology,Guangzhou,510006,China
7.University of Chinese Academy of Sciences,Beijing,100049,China
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GB/T 7714
Lin, Huaxing,Liu, Yuan,Wang, Zirui,et al. Enhanced CO2 Photoreduction through Spontaneous Charge Separation in End-Capping Assembly of Heterostructured Covalent-Organic Frameworks[J]. ANGEWANDTE CHEMIE - INTERNATIONAL EDITION,2022,61(50).
APA Lin, Huaxing.,Liu, Yuan.,Wang, Zirui.,Ling, Liying.,Huang, Hao.,...&Zhou, Tianhua.(2022).Enhanced CO2 Photoreduction through Spontaneous Charge Separation in End-Capping Assembly of Heterostructured Covalent-Organic Frameworks.ANGEWANDTE CHEMIE - INTERNATIONAL EDITION,61(50).
MLA Lin, Huaxing,et al."Enhanced CO2 Photoreduction through Spontaneous Charge Separation in End-Capping Assembly of Heterostructured Covalent-Organic Frameworks".ANGEWANDTE CHEMIE - INTERNATIONAL EDITION 61.50(2022).
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