固定式多酶级联的模块化,用于连续流动的酶选择性C-H氨基化
Weixi Kong1, Chen Huang1, Liya Zhou1
1School of Chemical Engineering and Technology, Hebei University of Technology, No. 8 Guangrong Road, Hongqiao District, 300130, Tianjin, China.
Angewandte Chemie (International ed. in English)
|June 13, 2024
概括
这项研究介绍了一种新的四种酶级联,用于对阿里拉尔干的酶选择性C-H氨基化,将批量化学物质转化为有价值的性氨基. 优化的流量系统显著提高了生产率和效率,为这一具有挑战性的合成转换.
科学领域:
- 合成化学 合成化学
- 生物催化剂是一种生物催化剂.
- 化学工程是化学工程的重要组成部分.
背景情况:
- 多酶级联 (MEC) 在合成化学中表现有前途,但缺乏可靠性.
- 对阿里拉尔干的酶选择性基C-H氨基化是一种具有挑战性的转化,用于产生高价值的性氨基.
研究的目的:
- 开发一种可靠的四种酶级联,用于酶选择性基基C-H氨基化.
- 通过共同固定和微环境调整来优化酶性能和系统生产力.
- 将布整合到连续气液细分流系统中.
主要方法:
- 构建一个四个酶级联,具有辅助因子独立和自我维持的双酶模块.
- 酶协同固定与微环境调用于模块优化.
- 集成到气液细分流系统中,用于连续处理.
主要成果:
- 使用低度NADH (0.5毫米) 实现了90%以上的转化,用于连续C-H氨基化阿里拉尔干 (高达100毫米).
- 获得了3.6g·L−1·h−1的高时空收益率 (STY),比之前的报道增加了90倍.
- 在酶性能,质量转移和系统兼容性方面同时改善.
结论:
- 开发的流量系统提供了一种强大而有效的方法,用于对酶选择性基C-H氨基化.
- 这种方法显著提高了合成奇拉胺胺的多酶级联的实用性和生产率.
- 该战略提供了一个可扩展的平台,用于从散装化学品中生产高价值的性胺.
相关概念视频
Reduction of Alkenes: Asymmetric Catalytic Hydrogenation
3.3K
Catalytic hydrogenation of alkenes is a transition-metal catalyzed reduction of the double bond using molecular hydrogen to give alkanes. The mode of hydrogen addition follows syn stereochemistry.
The metal catalyst used can be either heterogeneous or homogeneous. When hydrogenation of an alkene generates a chiral center, a pair of enantiomeric products is expected to form. However, an enantiomeric excess of one of the products can be facilitated using an enantioselective reaction or an...
The metal catalyst used can be either heterogeneous or homogeneous. When hydrogenation of an alkene generates a chiral center, a pair of enantiomeric products is expected to form. However, an enantiomeric excess of one of the products can be facilitated using an enantioselective reaction or an...
3.3K
Regioselectivity and Stereochemistry of Acid-Catalyzed Hydration
8.4K
The rate of acid-catalyzed hydration of alkenes depends on the alkene's structure, as the presence of alkyl substituents at the double bond can significantly influence the rate.
8.4K
Olefin Metathesis Polymerization: Acyclic Diene Metathesis (ADMET)
1.9K
Acyclic diene metathesis polymerization or ADMET polymerization involves cross-metathesis of terminal dienes, such as 1,8-nonadiene, to give linear unsaturated polymer and ethylene. As ADMET is a reversible process, the formed ethylene gas must be removed from the reaction mixture to complete the polymerization process.
Similar to cross-metathesis, ADMET also involves the formation of metallacyclobutane intermediate by [2+2] cycloaddition of one of the double bonds of a terminal diene with...
Similar to cross-metathesis, ADMET also involves the formation of metallacyclobutane intermediate by [2+2] cycloaddition of one of the double bonds of a terminal diene with...
1.9K
Introduction to Mechanisms of Enzyme Catalysis
8.1K
For many years, scientists thought that enzyme-substrate binding took place in a simple "lock-and-key" fashion. This model stated that the enzyme and substrate fit together perfectly in one instantaneous step. However, current research supports a more refined view scientists call induced fit. The induced-fit model expands upon the lock-and-key model by describing a more dynamic interaction between enzyme and substrate. As the enzyme and substrate come together, their interaction causes...
8.1K
Regioselectivity of Electrophilic Additions to Alkenes: Markovnikov's Rule
14.1K
If a set of reactants can yield multiple constitutional isomers, but one of the isomers is obtained as the major product, the reaction is said to be regioselective. In such reactions, bond formation or breaking is favored at one reaction site over others.
The hydrohalogenation of an unsymmetrical alkene can yield two haloalkane products, depending on which vinylic carbon takes up the halogen. However, one product usually predominates, where hydrogen adds to the vinylic carbon bearing the...
The hydrohalogenation of an unsymmetrical alkene can yield two haloalkane products, depending on which vinylic carbon takes up the halogen. However, one product usually predominates, where hydrogen adds to the vinylic carbon bearing the...
14.1K
Amines to Alkenes: Hofmann Elimination
2.5K
Alkenes can be obtained from amines via an E2 elimination. The amine is first converted into a good leaving group, such as a quaternary ammonium salt. This is accomplished by treating the amine with an excess of alkyl halide, which results in a halide salt. Next, the halide salt is transformed into a hydroxide salt that functions as a base to enable elimination.
Under thermal conditions, the hydroxide can abstract a proton from the β carbon; this generates an alkene with the simultaneous...
Under thermal conditions, the hydroxide can abstract a proton from the β carbon; this generates an alkene with the simultaneous...
2.5K


