Spatial Localization of Two Enzymes at Pickering Emulsion Droplet Interfaces for Cascade Reactions

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 localizi...

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Veröffentlicht in:Angewandte Chemie International Edition 2023-04, Vol.62 (15), p.e202300794-n/a
Hauptverfasser: Li, Ke, Zou, Houbing, Ettelaie, Rammile, Zhang, Jingxia, Yang, Hengquan
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Sprache:eng
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Zusammenfassung: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. Two different enzymes were precisely localized at the inner and outer interfaces of Pickering emulsion droplets with the aid of an asymmetrically modified mesoporous nanosheet. This unique system exhibited significantly enhanced cascading efficiency in oxidation reactions by creating reaction microenvironments appropriate for the different enzymes and enabling efficient intermediate transportation at the droplet interfaces.
ISSN:1433-7851
1521-3773
DOI:10.1002/anie.202300794