3D N-heterocyclic covalent organic frameworks for urea photosynthesis from NH3 and CO2
Abstract Artificial photosynthesis of urea from NH3 and CO2 seems to remain still essentially unexplored. Herein, three isomorphic three-dimensional covalent organic frameworks with twofold interpenetrated ffc topology are functionalized by benzene, pyrazine, and tetrazine active moieties, respectiv...
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| Format: | Article |
| Language: | English |
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Nature Portfolio
2025-01-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-025-56307-w |
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| author | Ning Li Jiale Zhang Xiangdong Xie Kang Wang Dongdong Qi Jiang Liu Ya-Qian Lan Jianzhuang Jiang |
| author_facet | Ning Li Jiale Zhang Xiangdong Xie Kang Wang Dongdong Qi Jiang Liu Ya-Qian Lan Jianzhuang Jiang |
| author_sort | Ning Li |
| collection | DOAJ |
| description | Abstract Artificial photosynthesis of urea from NH3 and CO2 seems to remain still essentially unexplored. Herein, three isomorphic three-dimensional covalent organic frameworks with twofold interpenetrated ffc topology are functionalized by benzene, pyrazine, and tetrazine active moieties, respectively. A series of experiment results disclose the gradually enhanced conductivity, light-harvesting capacity, photogenerated carrier separation efficiency, and co-adsorption capacity towards NH3 and CO2 in the order of benzene-, pyrazine-, and tetrazine-containing framework. This in turn endows tetrazine-containing framework with superior photocatalytic activity towards urea production from NH3 and CO2 with the yield of 523 μmol g−1 h−1, 40 and 4 times higher than that for benzene- and pyrazine-containing framework, respectively, indicating the heterocyclic N microenvironment-dependent catalytic performance for these three photocatalysts. This is further confirmed by in-situ spectroscopic characterization and density functional theory calculations. This work lays a way towards sustainable photosynthesis of urea. |
| format | Article |
| id | doaj-art-6eeae2d683a040518b0c0a3e795f6493 |
| institution | Kabale University |
| issn | 2041-1723 |
| language | English |
| publishDate | 2025-01-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj-art-6eeae2d683a040518b0c0a3e795f64932025-02-02T12:32:53ZengNature PortfolioNature Communications2041-17232025-01-0116111010.1038/s41467-025-56307-w3D N-heterocyclic covalent organic frameworks for urea photosynthesis from NH3 and CO2Ning Li0Jiale Zhang1Xiangdong Xie2Kang Wang3Dongdong Qi4Jiang Liu5Ya-Qian Lan6Jianzhuang Jiang7Beijing Key Laboratory for Science and Application of Functional Molecular and Crystalline Materials, Department of Chemistry and Chemical Engineering, School of Chemistry and Biological Engineering, University of Science and Technology BeijingBeijing Key Laboratory for Science and Application of Functional Molecular and Crystalline Materials, Department of Chemistry and Chemical Engineering, School of Chemistry and Biological Engineering, University of Science and Technology BeijingGuangdong Provincial Key Laboratory of Carbon Dioxide Resource Utilization, School of Chemistry, South China Normal UniversityBeijing Key Laboratory for Science and Application of Functional Molecular and Crystalline Materials, Department of Chemistry and Chemical Engineering, School of Chemistry and Biological Engineering, University of Science and Technology BeijingBeijing Key Laboratory for Science and Application of Functional Molecular and Crystalline Materials, Department of Chemistry and Chemical Engineering, School of Chemistry and Biological Engineering, University of Science and Technology BeijingGuangdong Provincial Key Laboratory of Carbon Dioxide Resource Utilization, School of Chemistry, South China Normal UniversityGuangdong Provincial Key Laboratory of Carbon Dioxide Resource Utilization, School of Chemistry, South China Normal UniversityBeijing Key Laboratory for Science and Application of Functional Molecular and Crystalline Materials, Department of Chemistry and Chemical Engineering, School of Chemistry and Biological Engineering, University of Science and Technology BeijingAbstract Artificial photosynthesis of urea from NH3 and CO2 seems to remain still essentially unexplored. Herein, three isomorphic three-dimensional covalent organic frameworks with twofold interpenetrated ffc topology are functionalized by benzene, pyrazine, and tetrazine active moieties, respectively. A series of experiment results disclose the gradually enhanced conductivity, light-harvesting capacity, photogenerated carrier separation efficiency, and co-adsorption capacity towards NH3 and CO2 in the order of benzene-, pyrazine-, and tetrazine-containing framework. This in turn endows tetrazine-containing framework with superior photocatalytic activity towards urea production from NH3 and CO2 with the yield of 523 μmol g−1 h−1, 40 and 4 times higher than that for benzene- and pyrazine-containing framework, respectively, indicating the heterocyclic N microenvironment-dependent catalytic performance for these three photocatalysts. This is further confirmed by in-situ spectroscopic characterization and density functional theory calculations. This work lays a way towards sustainable photosynthesis of urea.https://doi.org/10.1038/s41467-025-56307-w |
| spellingShingle | Ning Li Jiale Zhang Xiangdong Xie Kang Wang Dongdong Qi Jiang Liu Ya-Qian Lan Jianzhuang Jiang 3D N-heterocyclic covalent organic frameworks for urea photosynthesis from NH3 and CO2 Nature Communications |
| title | 3D N-heterocyclic covalent organic frameworks for urea photosynthesis from NH3 and CO2 |
| title_full | 3D N-heterocyclic covalent organic frameworks for urea photosynthesis from NH3 and CO2 |
| title_fullStr | 3D N-heterocyclic covalent organic frameworks for urea photosynthesis from NH3 and CO2 |
| title_full_unstemmed | 3D N-heterocyclic covalent organic frameworks for urea photosynthesis from NH3 and CO2 |
| title_short | 3D N-heterocyclic covalent organic frameworks for urea photosynthesis from NH3 and CO2 |
| title_sort | 3d n heterocyclic covalent organic frameworks for urea photosynthesis from nh3 and co2 |
| url | https://doi.org/10.1038/s41467-025-56307-w |
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