Modularization of Immobilized Multienzyme Cascades for Continuous-Flow Enantioselective C-H Amination.
Angew Chem Int Ed Engl
; 63(37): e202407778, 2024 Sep 09.
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 modules 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 100â
mM) utilizing the sole cofactor NADH (0.5â
mM) in >90 % conversion, achieving a high space-time yield (STY) of 3.6â
g â
L-1 â
h-1, which is a 90-fold increase over the highest value previously reported.
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Base de dados:
MEDLINE
Assunto principal:
Enzimas Imobilizadas
Idioma:
En
Ano de publicação:
2024
Tipo de documento:
Article