Applied Microbiology, Faculty of Biology and Biotechnology, Ruhr University Bochum, Universitätsstraße 150, 44780, Bochum, Germany.
Microbial Biotechnology, Faculty of Biology and Biotechnology, Ruhr University Bochum, Universitätsstraße 150, 44780, Bochum, Germany.
ChemSusChem. 2020 Apr 21;13(8):2072-2079. doi: 10.1002/cssc.201903438. Epub 2020 Mar 18.
Peroxidases and peroxygenases are promising classes of enzymes for biocatalysis because of their ability to carry out one-electron oxidation reactions and stereoselective oxyfunctionalizations. However, industrial application is limited, as the major drawback is the sensitivity toward the required peroxide substrates. Herein, we report a novel biocatalysis approach to circumvent this shortcoming: in situ production of H O by dielectric barrier discharge plasma. The discharge plasma can be controlled to produce hydrogen peroxide at desired rates, yielding desired concentrations. Using horseradish peroxidase, it is demonstrated that hydrogen peroxide produced by plasma treatment can drive the enzymatic oxidation of model substrates. Fungal peroxygenase is then employed to convert ethylbenzene to (R)-1-phenylethanol with an ee of >96 % using plasma-generated hydrogen peroxide. As direct treatment of the reaction solution with plasma results in reduced enzyme activity, the use of plasma-treated liquid and protection strategies are investigated to increase total turnover. Technical plasmas present a noninvasive means to drive peroxide-based biotransformations.
过氧化物酶和过氧酶是一类很有前途的酶，因为它们能够进行单电子氧化反应和立体选择性的氧化官能团化。然而，由于对所需过氧化物底物的敏感性，其工业应用受到限制。在此，我们报告了一种新的生物催化方法来克服这一缺点：通过介电阻挡放电等离子体原位生产 H2O2。可以控制放电等离子体以所需的速率产生过氧化氢，从而得到所需的浓度。使用辣根过氧化物酶，证明等离子体处理产生的过氧化氢可以驱动模型底物的酶促氧化。然后，使用真菌过氧酶，以超过 96%的对映体过量（ee）将乙苯转化为（R）-1-苯乙醇，使用等离子体产生的过氧化氢。由于直接用等离子体处理反应溶液会降低酶的活性，因此研究了使用等离子体处理过的液体和保护策略来提高总转化率。技术等离子体提供了一种非侵入性的方法来驱动基于过氧化物的生物转化。
