对映选择合成
胺化
辅因子
流动化学
化学
组合化学
级联
生物催化
还原胺化
级联反应
产量(工程)
立体化学
酶
有机化学
催化作用
色谱法
材料科学
反应机理
冶金
作者
Yanjun Jiang,Weixi Kong,Chen Huang,Liya Zhou,Jing Gao,Li Ma,Yunting Liu
标识
DOI:10.1002/ange.202407778
摘要
Multienzyme cascades (MECs) have gained much attention in synthetic chemistry but remain far from being a reliable synthetic tool. Here we report a four‐enzyme cascade comprising a cofactor‐independent and a cofactor self‐sustaining bienzymatic module for the enantioselective benzylic C‐H amination of arylalkanes, a challenging transformation from bulk chemicals to high value‐added chiral amines. The two modules were subsequently optimized by enzyme co‐immobilization with microenvironmental tuning, and finally integrated in a gas‐liquid segmented flow system, resulting in simultaneous improvements in enzyme performance, mass transfer, system compatibility, and productivity. The flow system enabled continuous C‐H amination of arylalkanes (up to 100 mM) utilizing the sole cofactor NADH (0.5 mM) in >90% conversion, achieving a high space‐time yield (STY) of 3.6 g·L ‐1 ·h ‐1 , which is a 90‐fold increase over previously reported values.
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