Dirks Tim, Stoesser Davina, Schüttler Steffen, Hollmann Frank, Golda Judith, Bandow Julia E
Applied Microbiology, Faculty of Biology and Biotechnology, Ruhr University Bochum, 44801, Bochum, Germany.
Plasma Interface Physics, Faculty of Physics and Astronomy, Ruhr University Bochum, 44801, Bochum, Germany.
ChemistryOpen. 2025 Sep;14(9):e202500057. doi: 10.1002/open.202500057. Epub 2025 Jun 22.
Plasma-generated HO can be used to fuel biocatalytic reactions that require HO as a cosubstrate, such as the conversion of ethylbenzene to (R)-1-phenylethanol ((R)-1-PhOl) catalyzed by unspecific peroxygenase from Agrocybe aegerita (rAaeUPO). Immobilization is recently shown to protect biocatalysts from inactivation by highly reactive plasma-produced species; however, HO supply by the employed plasma sources (μAPPJ and DBD) is limiting for rAaeUPO performance. This study evaluates a recently introduced capillary plasma jet for suitability to supply HO in situ. HO production is modulated by varying the water concentration in the feed gas, providing a greater operating window for applications in plasma-driven biocatalysis. In a static system after 80 min of biocatalysis, a turnover number of 44,199 mol mol is achieved without significant enzyme inactivation. By exchanging the reaction solution every 5 min, a total product yield of 122 μmol (R)-1-PhOl is achieved in 700 min run time, resulting in a total turnover number of 174,209 mol mol . This study concludes that the capillary plasma jet, due to its flexibility regarding feed gas, admixtures, and power input, is well suited for in situ HO generation for plasma-driven biocatalysis tailoring to enzymes with high HO turnover.
等离子体产生的羟基自由基(HO)可用于为需要HO作为共底物的生物催化反应提供燃料,例如由高大环柄菇(Agrocybe aegerita)的非特异性过氧合酶(rAaeUPO)催化乙苯转化为(R)-1-苯乙醇((R)-1-PhOl)。最近的研究表明,固定化可以保护生物催化剂不被高活性的等离子体产生的物质灭活;然而,所使用的等离子体源(μAPPJ和DBD)提供的HO对rAaeUPO的性能有限制。本研究评估了一种最近引入的毛细管等离子体射流用于原位供应HO的适用性。通过改变进料气体中的水浓度来调节HO的产生,为等离子体驱动的生物催化应用提供了更大的操作窗口。在静态系统中进行80分钟的生物催化后,实现了44,199 mol/mol的周转数,且酶没有明显失活。通过每5分钟更换一次反应溶液,在700分钟的运行时间内实现了122 μmol(R)-1-PhOl的总产物产量,总周转数为174,209 mol/mol。本研究得出结论,毛细管等离子体射流由于其在进料气体、添加剂和功率输入方面的灵活性,非常适合为等离子体驱动的生物催化原位产生HO,以适应具有高HO周转率的酶。