Enhancing photocatalytic efficiency through surface modification to manipulate internal electron-hole distribution
Abstract In this study, we synthesized ten g-C3N4-based covalent organic frameworks (COFs) and identified CN-306 as the most effective catalyst for visible-light-driven hydrogen peroxide (H2O2) production. Systematic optimization revealed that increasing ethanol proportions in the reaction medium si...
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| Format: | Article |
| Language: | English |
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Nature Portfolio
2025-05-01
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| Series: | npj Clean Water |
| Online Access: | https://doi.org/10.1038/s41545-025-00480-4 |
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| author | Hong Tu Bihong Tian Shunshun Chen Jingyi Xu Jianrong Yang Zhichao Zhao Shunhong Chen Jian Wu |
| author_facet | Hong Tu Bihong Tian Shunshun Chen Jingyi Xu Jianrong Yang Zhichao Zhao Shunhong Chen Jian Wu |
| author_sort | Hong Tu |
| collection | DOAJ |
| description | Abstract In this study, we synthesized ten g-C3N4-based covalent organic frameworks (COFs) and identified CN-306 as the most effective catalyst for visible-light-driven hydrogen peroxide (H2O2) production. Systematic optimization revealed that increasing ethanol proportions in the reaction medium significantly enhanced H2O2 yield, achieving a remarkable production rate of 5352 μmol g−1h−1 with a surface quantum efficiency of 7.27% at λ = 420 nm. Intriguingly, mechanistic investigations uncovered that excessive generation of singlet oxygen (1O2) acts as a critical inhibitory factor, impeding H2O2 accumulation. Multimodal characterization techniques combined with density functional theory (DFT) calculations were employed to unravel the origin of CN-306’s superior performance. Theoretical analyses demonstrated that CN-306 exhibits enhanced electron-hole separation efficiency, attributed to its reduced energy gap between the highest occupied molecular orbital (HOMO) and lowest unoccupied molecular orbital (LUMO), which facilitates photocarrier migration and suppresses detrimental recombination. Furthermore, this work elucidates the structure-function relationships governing site-specific functional group modifications in COFs and their profound influence on photocatalytic activity. These findings provide molecular-level insights into rational catalyst design for optimizing surface structures and advancing solar-driven H2O2 synthesis applications. |
| format | Article |
| id | doaj-art-0212ac61c635429ab49e508491b4e845 |
| institution | DOAJ |
| issn | 2059-7037 |
| language | English |
| publishDate | 2025-05-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | npj Clean Water |
| spelling | doaj-art-0212ac61c635429ab49e508491b4e8452025-08-20T03:16:33ZengNature Portfolionpj Clean Water2059-70372025-05-018111010.1038/s41545-025-00480-4Enhancing photocatalytic efficiency through surface modification to manipulate internal electron-hole distributionHong Tu0Bihong Tian1Shunshun Chen2Jingyi Xu3Jianrong Yang4Zhichao Zhao5Shunhong Chen6Jian Wu7State Key Laboratory of Green Pesticide, Guizhou UniversityState Key Laboratory of Green Pesticide, Guizhou UniversityState Key Laboratory of Green Pesticide, Guizhou UniversityState Key Laboratory of Green Pesticide, Guizhou UniversityState Key Laboratory of Green Pesticide, Guizhou UniversityState Key Laboratory of Green Pesticide, Guizhou UniversityState Key Laboratory of Green Pesticide, Guizhou UniversityState Key Laboratory of Green Pesticide, Guizhou UniversityAbstract In this study, we synthesized ten g-C3N4-based covalent organic frameworks (COFs) and identified CN-306 as the most effective catalyst for visible-light-driven hydrogen peroxide (H2O2) production. Systematic optimization revealed that increasing ethanol proportions in the reaction medium significantly enhanced H2O2 yield, achieving a remarkable production rate of 5352 μmol g−1h−1 with a surface quantum efficiency of 7.27% at λ = 420 nm. Intriguingly, mechanistic investigations uncovered that excessive generation of singlet oxygen (1O2) acts as a critical inhibitory factor, impeding H2O2 accumulation. Multimodal characterization techniques combined with density functional theory (DFT) calculations were employed to unravel the origin of CN-306’s superior performance. Theoretical analyses demonstrated that CN-306 exhibits enhanced electron-hole separation efficiency, attributed to its reduced energy gap between the highest occupied molecular orbital (HOMO) and lowest unoccupied molecular orbital (LUMO), which facilitates photocarrier migration and suppresses detrimental recombination. Furthermore, this work elucidates the structure-function relationships governing site-specific functional group modifications in COFs and their profound influence on photocatalytic activity. These findings provide molecular-level insights into rational catalyst design for optimizing surface structures and advancing solar-driven H2O2 synthesis applications.https://doi.org/10.1038/s41545-025-00480-4 |
| spellingShingle | Hong Tu Bihong Tian Shunshun Chen Jingyi Xu Jianrong Yang Zhichao Zhao Shunhong Chen Jian Wu Enhancing photocatalytic efficiency through surface modification to manipulate internal electron-hole distribution npj Clean Water |
| title | Enhancing photocatalytic efficiency through surface modification to manipulate internal electron-hole distribution |
| title_full | Enhancing photocatalytic efficiency through surface modification to manipulate internal electron-hole distribution |
| title_fullStr | Enhancing photocatalytic efficiency through surface modification to manipulate internal electron-hole distribution |
| title_full_unstemmed | Enhancing photocatalytic efficiency through surface modification to manipulate internal electron-hole distribution |
| title_short | Enhancing photocatalytic efficiency through surface modification to manipulate internal electron-hole distribution |
| title_sort | enhancing photocatalytic efficiency through surface modification to manipulate internal electron hole distribution |
| url | https://doi.org/10.1038/s41545-025-00480-4 |
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