Department of Systems Biotechnology, Konkuk University, 120 Neungdong-ro, Gwangjin-gu, Seoul, 050-29, South Korea.
Department of Chemistry, The Scripps Research Institute, 10550 N. Torrey Pines Road, La Jolla, CA, 92037, USA.
Angew Chem Int Ed Engl. 2021 Feb 15;60(7):3481-3486. doi: 10.1002/anie.202012658. Epub 2020 Dec 15.
We report a highly atom-efficient integrated cofactor/co-product recycling cascade employing cycloalkylamines as multifaceted starting materials for the synthesis of nylon building blocks. Reactions using E. coli whole cells as well as purified enzymes produced excellent conversions ranging from >80 and 95 % into desired ω-amino acids, respectively with varying substrate concentrations. The applicability of this tandem biocatalytic cascade was demonstrated to produce the corresponding lactams by employing engineered biocatalysts. For instance, ϵ-caprolactam, a valuable polymer building block was synthesized with 75 % conversion from 10 mM cyclohexylamine by employing whole-cell biocatalysts. This cascade could be an alternative for bio-based production of ω-amino acids and corresponding lactam compounds.
我们报告了一种高度原子经济的整合辅助因子/副产物回收级联反应，该反应使用环烷基胺作为多方面的起始原料，用于合成尼龙结构单元。使用大肠杆菌全细胞和纯化酶进行的反应在不同的底物浓度下，分别产生了出色的转化率，从 >80%到 95%不等，生成所需的ω-氨基酸。该串联生物催化级联反应的适用性通过使用工程化的生物催化剂来生产相应的内酰胺得到了证明。例如，ε-己内酰胺是一种有价值的聚合物结构单元，通过使用全细胞生物催化剂，从 10mM 环己胺合成，转化率为 75%。这种级联反应可能是生物基生产ω-氨基酸和相应内酰胺化合物的替代方法。
