Progress in Scaling up and Streamlining a Nanoconfined, Enzyme-Catalyzed Electrochemical Nicotinamide Recycling System for Biocatalytic Synthesis.
Progress in Scaling up and Streamlining a Nanoconfined, Enzyme-Catalyzed Electrochemical Nicotinamide Recycling System for Biocatalytic Synthesis.
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用于生物催化合成的纳米限制的酶催化电化学烟酰胺回收系统的放大和简化进展。
DOI：
10.1002/celc.202001166
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发表时间：
2020-11-16
期刊：
影响因子：
4
通讯作者：
Armstrong FA
中科院分区：
文献类型：
--
作者：
Cheng B;Wan L;Armstrong FA
电化学驱动的烟酰胺回收系统，被称为“电化学叶”，具有独特的属性，可适用于高价值化学品的小规模工业合成。一个完整的酶级联可以固定在纳米多孔电极的通道内，允许复杂的反应被通电，控制和监测连续真实的时间。该电极很容易通过将市售的氧化铟锡（ITO）纳米颗粒沉积在Ti载体上来制备，从而产生酶进入并结合的纳米孔网络。其中一种酶是光合黄素酶，铁氧还蛋白NADP+还原酶（FNR），其催化NADP（H）的准可逆电化学再循环并充当换能器。第二种酶是选择的任何NADP（H）依赖性脱氢酶，并且可以添加另外的酶以构建精细的级联反应，该级联反应通过NADP（H）在孔内的快速再循环而在氧化或还原方向上被驱动。在这篇文章中，我们描述了关键酶/辅因子参数的测量，以及从分析规模4 mL反应器（14 cm 2电极）到500 mL反应器（500 cm 2电极）的基本线性放大。 我们讨论的优点（可连接到计算机，天然酶固定化，低成本的电极和低辅因子的要求）和要解决的挑战（优化最低限度地使用酶应用于电极）。 从他们的书中抽出一片叶子：电化学叶子利用了在电极纳米孔内捕获的酶级联中操作的烟酰胺辅因子的快速高效电化学再生的发现。电极由市售的导电金属氧化物纳米颗粒制成。生物催化反应是同时通电，控制和监测。研究表明，将合成放大到反应器水平应该是简单的、具有成本效益的和“绿色”的。
An electrochemically driven nicotinamide recycling system, referred to as the ‘electrochemical leaf’ has unique attributes that may suit it to the small‐scale industrial synthesis of high‐value chemicals. A complete enzyme cascade can be immobilized within the channels of a nanoporous electrode, allowing complex reactions to be energized, controlled and monitored continuously in real time. The electrode is easily prepared by depositing commercially available indium tin oxide (ITO) nanoparticles on a Ti support, resulting in a network of nanopores into which enzymes enter and bind. One of the enzymes is the photosynthetic flavoenzyme, ferredoxin NADP+ reductase (FNR), which catalyzes the quasi‐reversible electrochemical recycling of NADP(H) and serves as the transducer. The second enzyme is any NADP(H)‐dependent dehydrogenase of choice, and further enzymes can be added to build elaborate cascades that are driven in either oxidation or reduction directions through the rapid recycling of NADP(H) within the pores. In this Article, we describe the measurement of key enzyme/cofactor parameters and an essentially linear scale‐up from an analytical scale 4 mL reactor with a 14 cm2 electrode to a 500 mL reactor with a 500 cm2 electrode. We discuss the advantages (energization, continuous monitoring that can be linked to a computer, natural enzyme immobilization, low costs of electrodes and low cofactor requirements) and challenges to be addressed (optimizing minimal use of enzyme applied to the electrode). Take a leaf out of their book: The electrochemical leaf exploits the discovery of rapid and highly efficient electrochemical regeneration of nicotinamide cofactors operating in enzyme cascades entrapped within electrode nanopores. The electrode is produced from commercially available conducting metal oxide nanoparticles. Biocatalytic reactions are simultaneously energized, controlled and monitored. Investigations show that the scale‐up of syntheses to reactor level should be simple, cost‐effective, and ‘green’.
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DOI：
10.1126/science.aac9283
发表时间：
2015-09-25
期刊：
Science (New York, N.Y.)
影响因子：
--
作者：
Mutti FG;Knaus T;Scrutton NS;Breuer M;Turner NJ
通讯作者：
Turner NJ
影响因子：
5.2
作者：
Broussy S;Cheloha RW;Berkowitz DB
通讯作者：
Berkowitz DB
影响因子：
4.5
作者：
Megarity, Clare F.;Siritanaratkul, Bhavin;Armstrong, Fraser A.
通讯作者：
Armstrong, Fraser A.
影响因子：
2.9
作者：
RIFE, JE;CLELAND, WW
通讯作者：
CLELAND, WW
影响因子：
3.5
作者：
Hanson, RL;Schwinden, MD;Szarka, LJ
通讯作者：
Szarka, LJ