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生物催化反应级联中三磷酸腺苷的电化学循环利用

Electrochemical Recycling of Adenosine Triphosphate in Biocatalytic Reaction Cascades.

作者信息

Ruccolo Serge, Brito Gilmar, Christensen Melodie, Itoh Tetsuji, Mattern Keith, Stone Kevin, Strotman Neil A, Sun Alexandra C

机构信息

Process Research and Development, Merck & Company Incorporated, Rahway, New Jersey 07065, United States.

出版信息

J Am Chem Soc. 2022 Dec 14;144(49):22582-22588. doi: 10.1021/jacs.2c08955. Epub 2022 Nov 30.

Abstract

Adenosine triphosphate (ATP) provides the driving force necessary for critical biological functions in all living organisms. In synthetic biocatalytic reactions, this cofactor is recycled using high-energy stoichiometric reagents, an approach that generates waste and poses challenges with enzyme stability. On the other hand, an electrochemical recycling system would use electrons as a convenient source of energy. We report a method that uses electricity to turn over enzymes for ATP generation in a simplified cellular respiration mimic. The method is simple, robust, and scalable, as well as broadly applicable to complex enzymatic processes including a four-enzyme biocatalytic cascade in the synthesis of the antiviral molnupiravir.

摘要

三磷酸腺苷(ATP)为所有生物体内关键的生物功能提供必要的驱动力。在合成生物催化反应中,这种辅因子通过使用高能化学计量试剂进行循环利用,这种方法会产生废物并对酶的稳定性构成挑战。另一方面,电化学循环系统将使用电子作为便捷的能量来源。我们报告了一种方法,该方法利用电力在简化的细胞呼吸模拟中使酶周转以生成ATP。该方法简单、稳健且可扩展,并且广泛适用于复杂的酶促过程,包括抗病毒药物莫努匹拉韦合成中的四酶生物催化级联反应。

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