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学者姓名：冯键强
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Abstract ：
Fluorinated compounds are scarce in nature, albeit they are in high demand in pharmaceuticals, agrochemicals, and materials. Fluorinated amides serve as prevalent structural motifs in pharmaceuticals and bioactive molecules. However, enantioselective synthesis of fluorinated amides remains challenging. Herein, we develop a visible-light-driven ene-reductase system that effectively generates carbon-centered radicals from fluorine-containing brominated amides. The system further enables their enantioselective hydroalkylation with alkenes, achieving high stereocontrol. Diversified alpha-fluorinated amides with high yield (up to 91%) and distal chirality (gamma-to F, up to 97% enantiomeric excess) are produced by optimizing the reaction system and performing enzyme engineering. This work advances photoenzymatic strategies for the integration of fluorinated chemical inputs and creates an opportunity for the asymmetric synthesis of valuable fluorinated compounds.
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| GB/T 7714 | Huang, Chaoqun , Jin, Xuerui , Liu, Zhenyu et al. Photoenzymatic enantioselective synthesis of fluorinated amides with remote stereocenter [J]. | NATURE COMMUNICATIONS , 2025 , 16 (1) . |
| MLA | Huang, Chaoqun et al. "Photoenzymatic enantioselective synthesis of fluorinated amides with remote stereocenter" . | NATURE COMMUNICATIONS 16 . 1 (2025) . |
| APA | Huang, Chaoqun , Jin, Xuerui , Liu, Zhenyu , Cui, Can , Zhang, Yang , Wang, Binju et al. Photoenzymatic enantioselective synthesis of fluorinated amides with remote stereocenter . | NATURE COMMUNICATIONS , 2025 , 16 (1) . |
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Abstract ：
Multicomponent reactions-those where three or more substrates combine into a product-have been highly useful in rapidly building chemical building blocks of increased complexity1, but achieving this enzymatically has remained rare2, 3, 4-5. This limitation primarily arises because an enzyme's active site is not typically set up to address multiple substrates, especially in cases involving multiple radical intermediates6. Recently, chemical catalytic radical sorting has emerged as an enabling strategy for a variety of useful reactions7,8. However, making such processes enantioselective is highly challenging owing to the inherent difficulty in the stereochemical control of radicals9. Here we repurpose a thiamine-dependent enzyme10,11 through directed evolution and combine it with photoredox catalysis to achieve a photobiocatalytic enantioselective three-component radical cross-coupling. This approach combines three readily available starting materials-aldehydes, alpha-bromo-carbonyls and alkenes-to give access to enantioenriched ketone products. Mechanistic investigations provide insights into how this dual photocatalyst-enzyme system precisely directs the three distinct radicals involved in the transformation, unlocking enzyme reactivity. Our approach has achieved exceptional stereoselectivity, with 24 out of 33 examples achieving >= 97% enantiomeric excess.
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| GB/T 7714 | Xing, Zhongqiu , Liu, Fulu , Feng, Jianqiang et al. Synergistic photobiocatalysis for enantioselective triple-radical sorting [J]. | NATURE , 2024 , 637 (8048) : 1118-, . |
| MLA | Xing, Zhongqiu et al. "Synergistic photobiocatalysis for enantioselective triple-radical sorting" . | NATURE 637 . 8048 (2024) : 1118-, . |
| APA | Xing, Zhongqiu , Liu, Fulu , Feng, Jianqiang , Yu, Lu , Wu, Zhouping , Zhao, Beibei et al. Synergistic photobiocatalysis for enantioselective triple-radical sorting . | NATURE , 2024 , 637 (8048) , 1118-, . |
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