Shanxi Key Laboratory of Coal-based Value-added Chemicals Green Catalysis Synthesis, School of Chemistry and Chemical Engineering, Shanxi University, Taiyuan, 030006, China.
Key Laboratory of Chemical Biology and Molecular Engineering of Ministry of Education, Institute of Molecular Science, Shanxi University, Taiyuan, 030006, China.
Angew Chem Int Ed Engl. 2023 Apr 3;62(15):e202300794. doi: 10.1002/anie.202300794. Epub 2023 Mar 3.
Developing biocatalytic cascades in abiological conditions is of utmost significance, but such processes often suffer from low reaction efficiency because of incompatible reaction environments and suppressed intermediate transportation. Herein we report a new type of biocatalytic cascade by localizing two different enzymes separately in the outer and inner interfacial layers of Pickering emulsion droplets. This versatile approach enables the localization of two enzymes in their preferred reaction microenvironments and simultaneously in nanoscale proximity of each other. The thus-designed interfacial biocatalytic cascades show outstanding catalytic efficiency in alkene epoxidation and thioether oxidation with in situ generation of hydrogen peroxide under mild conditions, 6.9-13.6 times higher than the catalytic efficiency of the free enzymes in solution and their multi-enzymatic counterparts. The remarkable interfacial effect of Pickering droplets was found to be responsible for the significantly enhanced cascading efficiency.
在非生物条件下开发生物催化级联反应至关重要，但由于反应环境不兼容和中间产物传输受到抑制，此类过程的反应效率往往较低。在此，我们报告了一种新的生物催化级联反应类型，即将两种不同的酶分别定位在 Pickering 乳液液滴的外界面层和内界面层中。这种多功能方法能够将两种酶定位在其各自优选的反应微环境中，同时彼此之间保持纳米级的接近。设计的界面生物催化级联反应在温和条件下用于烯烃环氧化和硫醚氧化，原位生成过氧化氢，其催化效率比溶液中游离酶和多酶体系分别高出 6.9-13.6 倍。发现 Pickering 液滴的显著界面效应是显著提高级联效率的原因。
