| Autor: |
Rui, Jinyan, Zhao, Qun, Huls, Anthony J., Soler, Jordi, Paris, Jared C., Chen, Zhenhong, Reshetnikov, Viktor, Yang, Yunfang, Guo, Yisong, Garcia-Borràs, Marc, Huang, Xiongyi |
| Jazyk: |
angličtina |
| Rok vydání: |
2022 |
| Předmět: |
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| Zdroj: |
Science |
| Popis: |
We report here the reprogramming of non-heme iron enzymes to catalyze an abiological C(sp(3))—H azidation reaction via iron-catalyzed radical relay. This biocatalytic transformation uses amidyl radicals as hydrogen atom abstractors and Fe(III)—N(3) intermediates as radical trapping agents. A high-throughput screening platform based on click chemistry was established for rapid optimization of the catalytic performance of enzymes identified. The final optimized variants function in whole Escherichia coli cells and deliver a range of azidation products with up to 10600 total turnovers and 93% enantiomeric excess. Given the high prevalence of radical relay reactions in organic synthesis and the large diversity of non-heme iron enzymes, we envision that this discovery will stimulate future development of metalloenzyme catalysts for synthetically useful transformations unexplored by natural evolution. |
| Databáze: |
OpenAIRE |
| Externí odkaz: |
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