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首页> 外文期刊>Catalysis science & technology >Morpholine-based buffers activate aerobic photobiocatalysis via spin correlated ion pair formation
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Morpholine-based buffers activate aerobic photobiocatalysis via spin correlated ion pair formation

机译：Morpholine-based缓冲区激活有氧photobiocatalysis通过离子对自旋相关形成

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摘要

The use of enzymes for synthetic applications is a powerful and environmentally-benign approach to increase molecular complexity. Oxidoreductases selectively introduce oxygen and hydrogen atoms into myriad substrates, catalyzing the synthesis of chemical and pharmaceutical building blocks for chemical production. However, broader application of this class of enzymes is limited by the requirements of expensive cofactors and low operational stability. Herein, we show that morpholine-based buffers, especially 3-(N-morpholino)propanesulfonic acid (MOPS), promote photoinduced flavoenzyme-catalyzed asymmetric redox transformations by regenerating the flavin cofactor via sacrificial electron donation and by increasing the operational stability of flavin-dependent oxidoreductases. The stabilization of the active forms of flavin by MOPS via formation of the spin correlated ion pair (3)[flavin(-)-MOPS+] ensemble reduces the formation of hydrogen peroxide, circumventing the oxygen dilemma under aerobic conditions detrimental to fragile enzymes.
机译：使用酶的合成是一个应用程序强大和环保性双重方法增加分子的复杂性。有选择地介绍原子氧和氢到无数的基质,催化合成化学和制药的构建块化工生产。这类酶的应用是有限的昂贵的代数余子式和要求较低的操作稳定性。morpholine-based缓冲区,尤其是(3) - N-morpholino propanesulfonic酸(拖把),促进光诱导的flavoenzyme-catalyzed不对称氧化还原再生的转换通过牺牲黄素代数余子式电子捐赠和通过增加操作稳定flavin-dependent氧化还原酶。稳定的活性形式的黄素拖把通过自旋相关离子的形成对(3)[黄素(-)拖把+]整体降低了过氧化氢的形成,绕过在有氧条件下氧气的困境损害脆弱的酶。

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