COFcap2, a recyclable tandem catalysis reactor for nitrogen fixation and conversion to chiral amines
Abstract Two or more catalysts conducting multistep reactions in the same reactor, concurrent tandem catalysis, could enable (bio)pharmaceutical and fine chemical manufacturing to become much more sustainable. Herein we report that co-immobilization of metal nanoparticles and a biocatalytic system w...
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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/s41467-025-56214-0 |
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| author | Qianqian Zhu Peijie Dong Jiangyue Yu Zhifang Wang Ting Wang Shan Qiao Jinjin Liu Shubo Geng Yunlong Zheng Peng Cheng Michael J. Zaworotko Zhenjie Zhang Yao Chen |
| author_facet | Qianqian Zhu Peijie Dong Jiangyue Yu Zhifang Wang Ting Wang Shan Qiao Jinjin Liu Shubo Geng Yunlong Zheng Peng Cheng Michael J. Zaworotko Zhenjie Zhang Yao Chen |
| author_sort | Qianqian Zhu |
| collection | DOAJ |
| description | Abstract Two or more catalysts conducting multistep reactions in the same reactor, concurrent tandem catalysis, could enable (bio)pharmaceutical and fine chemical manufacturing to become much more sustainable. Herein we report that co-immobilization of metal nanoparticles and a biocatalytic system within a synthetic covalent organic framework capsule, COFcap-2, functions like an artificial cell in that, whereas the catalysts are trapped within 300-400 nm cavities, substrates/products can ingress/egress through ca. 2 nm windows. The COFcap-2 reactor is first coated onto an electrode surface and then used to prepare eleven homochiral amines using dinitrogen as a feedstock. The amines, including drug product intermediates and active pharmaceutical ingredient, are prepared in >99% enantiomeric excess under ambient conditions in water. Importantly, the COFcap-2 system is recycled 15 times with retention of performance, addressing the relative instability and poor recyclability of enzymes that has hindered their broad implementation for energy-efficient, low waste production of chemicals and (bio)pharmaceuticals. |
| format | Article |
| id | doaj-art-bd567a6a50774555aca5c9b51228ed19 |
| institution | Kabale University |
| issn | 2041-1723 |
| language | English |
| publishDate | 2025-01-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj-art-bd567a6a50774555aca5c9b51228ed192025-01-26T12:42:33ZengNature PortfolioNature Communications2041-17232025-01-011611910.1038/s41467-025-56214-0COFcap2, a recyclable tandem catalysis reactor for nitrogen fixation and conversion to chiral aminesQianqian Zhu0Peijie Dong1Jiangyue Yu2Zhifang Wang3Ting Wang4Shan Qiao5Jinjin Liu6Shubo Geng7Yunlong Zheng8Peng Cheng9Michael J. Zaworotko10Zhenjie Zhang11Yao Chen12State Key Laboratory of Medicinal Chemical Biology, College of Chemistry, Nankai UniversityCollege of Pharmacy, Nankai UniversityCollege of Pharmacy, Nankai UniversityState Key Laboratory of Medicinal Chemical Biology, College of Chemistry, Nankai UniversityState Key Laboratory of Medicinal Chemical Biology, College of Chemistry, Nankai UniversityCollege of Pharmacy, Nankai UniversityState Key Laboratory of Medicinal Chemical Biology, College of Chemistry, Nankai UniversityState Key Laboratory of Medicinal Chemical Biology, College of Chemistry, Nankai UniversityCollege of Pharmacy, Nankai UniversityState Key Laboratory of Medicinal Chemical Biology, College of Chemistry, Nankai UniversityDepartment of Chemical Sciences, Bernal Institute, University of Limerick, LimerickState Key Laboratory of Medicinal Chemical Biology, College of Chemistry, Nankai UniversityState Key Laboratory of Medicinal Chemical Biology, College of Chemistry, Nankai UniversityAbstract Two or more catalysts conducting multistep reactions in the same reactor, concurrent tandem catalysis, could enable (bio)pharmaceutical and fine chemical manufacturing to become much more sustainable. Herein we report that co-immobilization of metal nanoparticles and a biocatalytic system within a synthetic covalent organic framework capsule, COFcap-2, functions like an artificial cell in that, whereas the catalysts are trapped within 300-400 nm cavities, substrates/products can ingress/egress through ca. 2 nm windows. The COFcap-2 reactor is first coated onto an electrode surface and then used to prepare eleven homochiral amines using dinitrogen as a feedstock. The amines, including drug product intermediates and active pharmaceutical ingredient, are prepared in >99% enantiomeric excess under ambient conditions in water. Importantly, the COFcap-2 system is recycled 15 times with retention of performance, addressing the relative instability and poor recyclability of enzymes that has hindered their broad implementation for energy-efficient, low waste production of chemicals and (bio)pharmaceuticals.https://doi.org/10.1038/s41467-025-56214-0 |
| spellingShingle | Qianqian Zhu Peijie Dong Jiangyue Yu Zhifang Wang Ting Wang Shan Qiao Jinjin Liu Shubo Geng Yunlong Zheng Peng Cheng Michael J. Zaworotko Zhenjie Zhang Yao Chen COFcap2, a recyclable tandem catalysis reactor for nitrogen fixation and conversion to chiral amines Nature Communications |
| title | COFcap2, a recyclable tandem catalysis reactor for nitrogen fixation and conversion to chiral amines |
| title_full | COFcap2, a recyclable tandem catalysis reactor for nitrogen fixation and conversion to chiral amines |
| title_fullStr | COFcap2, a recyclable tandem catalysis reactor for nitrogen fixation and conversion to chiral amines |
| title_full_unstemmed | COFcap2, a recyclable tandem catalysis reactor for nitrogen fixation and conversion to chiral amines |
| title_short | COFcap2, a recyclable tandem catalysis reactor for nitrogen fixation and conversion to chiral amines |
| title_sort | cofcap2 a recyclable tandem catalysis reactor for nitrogen fixation and conversion to chiral amines |
| url | https://doi.org/10.1038/s41467-025-56214-0 |
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