基于台式 NMR 的非对映选择性酶法 α 氨基酸合成在线分析:定量与验证

IF 3.1 3区 化学 Q2 CHEMISTRY, APPLIED
Luca F. Schmidt, Logia Jolly, Leon Hennecke, Fernando Lopez Haro, Harald Gröger and Andreas Liese*, 
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引用次数: 0

摘要

本研究调查了商用低场台式 NMR 在实时监测酶催化反应中的应用,重点是苏氨酸醛缩酶催化的甘氨酸和苯甲醛之间立体选择性醛缩反应的非对映选择性。尽管台式核磁共振系统的微弱电磁场会造成固有的信号重叠,但一种互补的硬建模(CHM)方法可有效区分非对映异构体,从而确定酶的非对映选择性,并实现从动力学控制到热力学控制的过渡。在线核磁共振分析显示非对映异构体的过量率为 37:63(赤/赤),这与通过气相色谱和高效液相色谱进行的离线测量结果(36:64)非常吻合。利用 CHM 测定非对映异构体提高了酶促反应在线监测的效率,有望在制药工艺开发方面取得重大进展。总之,这项研究强调了台式 NMR 系统在酶促反应在线分析中的实用性,为深入了解反应机理、选择性和平衡动态提供了依据,从而促进了精细化工领域更高效的工艺优化。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Benchtop NMR-Based In-Line Analysis of Diastereoselective Enzymatic α-Amino Acid Synthesis: Quantification and Validation

This study investigates the application of a commercial low-field benchtop NMR for real-time monitoring of enzymatically catalyzed reactions, focusing on the diastereoselectivity of the threonine aldolase-catalyzed stereoselective aldol reaction between glycine and benzaldehyde. Despite the signal overlap inherent in the weak electromagnetic field of the benchtop NMR system, a complemental hard modeling (CHM) approach effectively differentiates between diastereomers, enabling the determination of enzymatic diastereoselectivity and the transition from kinetic to thermodynamic control. In particular, the achievement of thermodynamic equilibrium in the enzymatic aldol reaction is observed for the first time using in-line methods, occurring at 30% benzaldehyde conversion after 2 h. In-line NMR analysis reveals a diastereomeric excess of 37:63 (erythro/threo), which closely aligns with off-line measurements via GC and HPLC (36:64). This determination of diastereomers using CHM enhances the efficiency of in-line monitoring in enzymatic reactions, promising significant advancements in pharmaceutical process development. Overall, the study underscores the utility of benchtop NMR systems for in-line analysis of enzymatic reactions, offering insights into reaction mechanisms, selectivity, and equilibrium dynamics, thereby facilitating more efficient process optimization in the area of fine chemicals.

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来源期刊
CiteScore
6.90
自引率
14.70%
发文量
251
审稿时长
2 months
期刊介绍: The journal Organic Process Research & Development serves as a communication tool between industrial chemists and chemists working in universities and research institutes. As such, it reports original work from the broad field of industrial process chemistry but also presents academic results that are relevant, or potentially relevant, to industrial applications. Process chemistry is the science that enables the safe, environmentally benign and ultimately economical manufacturing of organic compounds that are required in larger amounts to help address the needs of society. Consequently, the Journal encompasses every aspect of organic chemistry, including all aspects of catalysis, synthetic methodology development and synthetic strategy exploration, but also includes aspects from analytical and solid-state chemistry and chemical engineering, such as work-up tools,process safety, or flow-chemistry. The goal of development and optimization of chemical reactions and processes is their transfer to a larger scale; original work describing such studies and the actual implementation on scale is highly relevant to the journal. However, studies on new developments from either industry, research institutes or academia that have not yet been demonstrated on scale, but where an industrial utility can be expected and where the study has addressed important prerequisites for a scale-up and has given confidence into the reliability and practicality of the chemistry, also serve the mission of OPR&D as a communication tool between the different contributors to the field.
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