Insights into excitonic behavior in single-atom covalent organic frameworks for efficient photo-Fenton-like pollutant degradation
Abstract The generation of radicals through photo-Fenton-like reactions demonstrates significant potential for remediating emerging organic contaminants (EOCs) in complex aqueous environments. However, the excitonic effect, induced by Coulomb interactions between photoexcited electrons and holes, re...
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Nature Portfolio
2025-01-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-025-56103-6 |
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| author | Chao Zhu Mingzheng Yang Bo Jiang Lun Lu Qile Fang Yong Zheng Shuang Song Baoliang Chen Yi Shen |
| author_facet | Chao Zhu Mingzheng Yang Bo Jiang Lun Lu Qile Fang Yong Zheng Shuang Song Baoliang Chen Yi Shen |
| author_sort | Chao Zhu |
| collection | DOAJ |
| description | Abstract The generation of radicals through photo-Fenton-like reactions demonstrates significant potential for remediating emerging organic contaminants (EOCs) in complex aqueous environments. However, the excitonic effect, induced by Coulomb interactions between photoexcited electrons and holes, reduces carrier utilization efficiency in these systems. In this study, we develop Cu single-atom-loaded covalent organic frameworks (CuSA/COFs) as models to modulate excitonic effects. Temperature-dependent photoluminescence and ultrafast transient absorption spectra reveal that incorporating acenaphthene units into the linker (CuSA/Ace-COF) significantly reduces exciton binding energy (E b). This modification not only enhances peroxymonosulfate adsorption at Cu active sites but also facilitates rapid electron transfer and promotes selective hydroxyl radical generation. Compared to CuSA/Obq-COF (E b = 25.6 meV), CuSA/Ace-COF (E b = 12.2 meV) shows a 39.5-fold increase in the pseudo-first-order rate constant for sulfamethoxazole degradation (0.434 min−1). This work provides insights into modulating excitonic behavior in single-atom catalysts via linker engineering for EOCs degradation. |
| format | Article |
| id | doaj-art-875f88536ce5413ca078cf7b42429218 |
| institution | Kabale University |
| issn | 2041-1723 |
| language | English |
| publishDate | 2025-01-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj-art-875f88536ce5413ca078cf7b424292182025-01-19T12:31:29ZengNature PortfolioNature Communications2041-17232025-01-0116111310.1038/s41467-025-56103-6Insights into excitonic behavior in single-atom covalent organic frameworks for efficient photo-Fenton-like pollutant degradationChao Zhu0Mingzheng Yang1Bo Jiang2Lun Lu3Qile Fang4Yong Zheng5Shuang Song6Baoliang Chen7Yi Shen8Department of Environment, Zhejiang University of TechnologyDepartment of Environment, Zhejiang University of TechnologyDepartment of Environment, Zhejiang University of TechnologyState Environmental Protection Key Laboratory of Environmental Pollution Health Risk Assessment Ministry of Ecology and Environment, South China Institute of Environmental SciencesAdvanced Institute of Natural Sciences, Beijing Normal University at ZhuhaiCollege of Materials and Chemical Engineering, China Three Gorges UniversityDepartment of Environment, Zhejiang University of TechnologyFaculty of Agriculture, Life, and Environmental Sciences and Department of Environmental Science, Zhejiang UniversityDepartment of Environment, Zhejiang University of TechnologyAbstract The generation of radicals through photo-Fenton-like reactions demonstrates significant potential for remediating emerging organic contaminants (EOCs) in complex aqueous environments. However, the excitonic effect, induced by Coulomb interactions between photoexcited electrons and holes, reduces carrier utilization efficiency in these systems. In this study, we develop Cu single-atom-loaded covalent organic frameworks (CuSA/COFs) as models to modulate excitonic effects. Temperature-dependent photoluminescence and ultrafast transient absorption spectra reveal that incorporating acenaphthene units into the linker (CuSA/Ace-COF) significantly reduces exciton binding energy (E b). This modification not only enhances peroxymonosulfate adsorption at Cu active sites but also facilitates rapid electron transfer and promotes selective hydroxyl radical generation. Compared to CuSA/Obq-COF (E b = 25.6 meV), CuSA/Ace-COF (E b = 12.2 meV) shows a 39.5-fold increase in the pseudo-first-order rate constant for sulfamethoxazole degradation (0.434 min−1). This work provides insights into modulating excitonic behavior in single-atom catalysts via linker engineering for EOCs degradation.https://doi.org/10.1038/s41467-025-56103-6 |
| spellingShingle | Chao Zhu Mingzheng Yang Bo Jiang Lun Lu Qile Fang Yong Zheng Shuang Song Baoliang Chen Yi Shen Insights into excitonic behavior in single-atom covalent organic frameworks for efficient photo-Fenton-like pollutant degradation Nature Communications |
| title | Insights into excitonic behavior in single-atom covalent organic frameworks for efficient photo-Fenton-like pollutant degradation |
| title_full | Insights into excitonic behavior in single-atom covalent organic frameworks for efficient photo-Fenton-like pollutant degradation |
| title_fullStr | Insights into excitonic behavior in single-atom covalent organic frameworks for efficient photo-Fenton-like pollutant degradation |
| title_full_unstemmed | Insights into excitonic behavior in single-atom covalent organic frameworks for efficient photo-Fenton-like pollutant degradation |
| title_short | Insights into excitonic behavior in single-atom covalent organic frameworks for efficient photo-Fenton-like pollutant degradation |
| title_sort | insights into excitonic behavior in single atom covalent organic frameworks for efficient photo fenton like pollutant degradation |
| url | https://doi.org/10.1038/s41467-025-56103-6 |
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