Biocompatible a-Methylenation of Metabolic Butyraldehyde in Living Bacteria
Biocompatible a-Methylenation of Metabolic Butyraldehyde in Living Bacteria
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活细菌中代谢丁醛的生物相容性α-甲基化
DOI：
10.1002/ange.202306347
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发表时间：
2023
影响因子：
--
通讯作者：
Dennis J
中科院分区：
文献类型：
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作者：
Dennis J
小分子有机催化剂在所有生物体中都很丰富。然而，它们在细胞中作为有机催化剂的用途还未得到充分探索。在这里，我们报告说，有机催化的羟醛化学可以与活的大肠杆菌连接，使细胞醛的α-亚甲基化使用生物胺，如L-Pro或磷酸盐。生物相容性反应是温和的，并且可以通过工程代谢与由D-葡萄糖产生的丁醛相结合，从而能够通过厌氧发酵生产2-亚甲基丁醛（2-MB）和2-甲基丁醛（2-MBA），以及通过全细胞催化生产2-甲基丁醇（2-MBO）。总体而言，本研究证明了非酶促有机催化和体内代谢反应的组合，用于可持续合成仅使用酶化学无法获得的有价值的非天然化学品。
Small molecule organocatalysts are abundant in all living organisms. However, their use as organocatalysts in cells has been underexplored. Herein, we report that organocatalytic aldol chemistry can be interfaced with livingEscherichia colito enable the α‐methylenation of cellular aldehydes using biogenic amines such as L‐Pro or phosphate. The biocompatible reaction is mild and can be interfaced with butyraldehyde generated from D‐glucose via engineered metabolism to enable the production of 2‐methylenebutanal (2‐MB) and 2‐methylbutanal (2‐MBA) by anaerobic fermentation, and 2‐methylbutanol (2‐MBO) by whole‐cell catalysis. Overall, this study demonstrates the combination of non‐enzymatic organocatalytic and metabolic reactions in vivo for the sustainable synthesis of valuable non‐natural chemicals that cannot be accessed using enzymatic chemistry alone.