Department of Physics, Chemistry and Pharmacy, University of Southern Denmark, Campusvej 55, 5230, Odense, Denmark.
Institute of Chemistry and Biochemistry, Freie Universität Berlin, Takustr. 3, 14195, Berlin, Germany.
Angew Chem Int Ed Engl. 2021 Apr 6;60(15):8410-8414. doi: 10.1002/anie.202013737. Epub 2021 Mar 5.
Multienzyme cascade biocatalysis is an efficient synthetic process, avoiding the isolation/purification of intermediates and shifting the reaction equilibrium to the product side.. However, multienzyme systems are often limited by their incompatibility and cross-reactivity. Herein, we report a multi-responsive emulsion to proceed multienzyme reactions sequentially for high reactivity. The emulsion is achieved using a CO , pH, and thermo-responsive block copolymer as a stabilizer, allowing the on-demand control of emulsion morphology and phase composition. Applying this system to a three-step cascade reaction enables the individual optimal condition for each enzyme, and a high overall conversion (ca. 97 % of the calculated limit) is thereby obtained. Moreover, the multi-responsiveness of the emulsion allows the facile and separate yielding/recycling of products, polymers and active enzymes. Besides, the system could be scaled up with a good yield.
多酶级联生物催化是一种有效的合成过程,避免了中间产物的分离/纯化,并将反应平衡推向产物侧。然而,多酶体系通常受到其不兼容性和交叉反应性的限制。在此,我们报告了一种多响应乳液,用于顺序进行多酶反应以获得高反应性。乳液是使用 CO 2 、pH 值和温敏嵌段共聚物作为稳定剂来实现的,允许按需控制乳液形态和相组成。将该体系应用于三步级联反应中,可以使每个酶都处于最佳条件下,从而获得高的总转化率(约为计算极限的 97%)。此外,乳液的多响应性允许产物、聚合物和活性酶的轻松分离回收。此外,该体系可以很好地放大规模,收率良好。