Department of Chemistry and Biochemistry, University of South Carolina, 631 Sumter Street, Columbia, SC 29208, USA.
Department of Chemistry and Biochemistry, University of South Carolina, 631 Sumter Street, Columbia, SC 29208, USA; Department of Chemical and Biochemical Engineering, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, Fujian, China.
Bioresour Technol. 2020 Sep;311:123538. doi: 10.1016/j.biortech.2020.123538. Epub 2020 May 15.
Cytochrome P450 OleT is a fatty acid decarboxylase that uses hydrogen peroxide (HO) to catalyze the production of terminal alkenes, which are industrially important chemicals with biofuel and synthetic applications. Despite its requirement for large turnover levels, high concentrations of HO may cause heme group degradation, diminishing enzymatic activity and limiting broad application for synthesis. Here, we report an artificial enzyme cascade composed of glucose oxidase (GOx) and OleT from Staphylococcus aureus for efficient terminal alkene production. By adjusting the ratio of GOx to OleT, the GOx-based tandem catalysis shows significantly improved product yield compared to the HO injection method. Moreover, the co-assembly of the GOx/OleT enzymes with a polymer, forming polymer-dual enzymes nanoparticles, displays improved activity compared to the free enzyme. This dual strategy provides a simple and efficient system to transform a naturally abundant feedstock to industrially important chemicals.
细胞色素 P450 OleT 是一种脂肪酸脱羧酶，它使用过氧化氢 (HO) 来催化末端烯烃的生成，这些末端烯烃是具有生物燃料和合成应用的工业重要化学品。尽管它需要高的周转率水平，但高浓度的 HO 可能导致血红素基团降解，降低酶的活性，并限制其在合成中的广泛应用。在这里，我们报告了一种由葡萄糖氧化酶 (GOx) 和来自金黄色葡萄球菌的 OleT 组成的人工酶级联，用于高效生产末端烯烃。通过调整 GOx 与 OleT 的比例，基于 GOx 的串联催化与 HO 注射法相比，产物产率显著提高。此外，GOx/OleT 酶与聚合物共组装，形成聚合物双重酶纳米颗粒，与游离酶相比显示出更高的活性。这种双重策略提供了一种简单有效的系统，可以将天然丰富的原料转化为工业上重要的化学品。
