Combination of bio- and chemocatalysis for dynamic kinetic resolution: The assembly strategies for nanozeolite-modified flow microchannel reactors

• Published in: Journal of catalysis Vol. 300; pp. 1 - 8
• Main Authors: Wang, Zhoujun, Li, Xiang, Wang, Wanlu, Tang, Yi, Zhang, Yahong
• Format: Journal Article
• Language: English
• Published: Amsterdam Elsevier Inc 01-04-2013; Elsevier; Elsevier BV
• Subjects: active sites; Assembly; Biological and medical sciences; Catalysis; catalysts; Chemistry; Chemoenzyme catalysis; enzymes; Exact sciences and technology; Fundamental and applied biological sciences. Psychology; General and physical chemistry; immobilized enzymes; Ion-exchange; Mechanisms. Catalysis. Electron transfer. Models; Microchannel reactor; Molecular biophysics; Nanocrystals; Nanozeolite; Physical chemistry in biology; Reaction kinetics; strategies; Surface physical chemistry; Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry; zeolites; Zeolites: preparations and properties; Nanozeolite; Microchannel reactor; Chemoenzyme catalysis; Assembly; Catalytic reaction; Enzymatic catalysis; Zeolite; Heterogeneous catalysis; Dynamics; Kinetics; Reactor; Immobilized enzyme; Nanocrystal
• ISSN: 0021-9517; 1090-2694
• DOI: 10.1016/j.jcat.2012.12.008

Three assembly strategies for combining bio- and chemocatalysis for one-pot dynamic kinetic resolution (DKR) based upon nanozeolite-modified flow microchannel reactors (MCR), listed as co-assembled MCR (a), segment-assembled MCR (b), and region-assembled MCR (c), are performed and discussed. The one-pot DKR process of the sec-alcohol can be accomplished quickly and highly selectively in the flow MCR under the optimum assembly design within 30min. [Display omitted]
► Nanozeolite-modified MCR is employed for the one-pot combination of bio- and chemocatalysts. ► Three assembly strategies in such MCR are proposed to develop the one-pot DKR of 1-PE. ► Three assembly strategies display different compatibilities for different active centers. ► The optimum DKR of 1-PE achieves 97% conversion and 99% selectivity in 30min.
The combination of bio- and chemocatalysts in one-pot is regarded as a breakthrough both for development of new catalytic concepts and for preparation of high-value chemicals. Zeolite nanocrystals (nanozeolites) have been proved as the most used chemical catalysts and as promising supports for enzyme immobilization. These capabilities of nanozeolites endow them with new possibilities for constructing desired platforms for the combination of bio- and chemocatalysis. In this article, several strategies are proposed to develop a one-pot flow microchannel reactor (MCR) by combining enzyme and chemocatalysis via a nanozeolite assembly approach, and the compatibilities of different types of active centers in various assembly strategies are systematically discussed on the basis of the catalytic results of dynamic kinetic resolution (DKR) of sec-alcohol. By precisely controlling the spatial distribution and the ratio of acidic and enzymatic active sites, as well as the reaction conditions, nanozeolite-modified MCR can achieve fast and highly selective one-pot DKR of sec-alcohol within 30min.