Modularization of Immobilized Multienzyme Cascades for Continuous-Flow Enantioselective C-H Amination.
Angew Chem Int Ed Engl
; : e202407778, 2024 Jun 13.
Article
em En
| MEDLINE
| ID: mdl-38871651
ABSTRACT
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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Coleções:
01-internacional
Base de dados:
MEDLINE
Idioma:
En
Revista:
Angew Chem Int Ed Engl
Ano de publicação:
2024
Tipo de documento:
Article