Highly Productive Oxidative Biocatalysis in Continuous Flow by Enhancing the Aqueous Equilibrium Solubility of Oxygen

Highly Productive Oxidative Biocatalysis in Continuous Flow by Enhancing the Aqueous Equilibrium Solubility of Oxygen
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DOI:
10.1002/anie.201803675
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发表时间:
2018-08-13
影响因子:
16.6
通讯作者:
Blacker, A. John
Blacker, A. John
中科院分区:
化学1区
文献类型:
--
作者:
Chapman, Michael R.;Cosgrove, Sebastian C.;Blacker, A. John

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我们报告了一种简单、温和和合成清洁的方法,与传统的间歇式气/液系统相比,可以将酶氧化反应的速度加快高达100倍。生物催化分解双氧水直接在反应介质中产生可溶的O-2源,从而使水中O-2的浓度在安全和实用的条件下增加到超过平衡溶解度。为了更好地利用这种方法,开发了一种新型的流动反应器,以最大限度地提高生产率(g产物L(-1)h(-1))。这种可扩展的台式方法与传统的生物氧化方法相比具有明显的优势,因为它不需要使用加压气体或专门的设备。该方法适用于不同的氧化物酶,并与各种官能团兼容。这些结果最终产生了创纪录的生物氧化时空产率。
We report a simple, mild, and synthetically clean approach to accelerate the rate of enzymatic oxidation reactions by a factor of up to 100 when compared to conventional batch gas/liquid systems. Biocatalytic decomposition of H2O2 is used to produce a soluble source of O-2 directly in reaction media, thereby enabling the concentration of aqueous O-2 to be increased beyond equilibrium solubility under safe and practical conditions. To best exploit this method, a novel flow reactor was developed to maximize productivity (g product L(-1)h(-1)). This scalable benchtop method provides a distinct advantage over conventional bio-oxidation in that no pressurized gas or specialist equipment is employed. The method is general across different oxidase enzymes and compatible with a variety of functional groups. These results culminate in record space-time yields for bio-oxidation.