Ionic liquid droplet micro-reactor for catalysis reactions not at equilibrium

Zhang, Ming; Ettelaie, Rammile; Yan, Tao; Zhang, Suojiang; Cheng, Fangqin; Binks, Bernard P.; Yang, Hengquan

Abstract

We develop a novel strategy to more effectively and controllably process continuous enzymatic or homogeneous catalysis reactions based on non-aqueous Pickering emulsions. A key element of this strategy is “bottom-up” construction of a macroscale continuous flow reaction system through packing catalyst-containing micron-sized ionic liquid (IL) droplets in oil in a column reactor. Due to the continuous influx of reactants into the droplets and the continuous release of products from the droplets, catalysis reactions in such a system can take place without limitations arising from establishment of the reaction equilibrium and catalyst separation, inherent in conventional batch reactions. As proof of the concept, enzymatic enantioselective trans-esterification and CuI-catalyzed cycloaddition reactions using this IL droplet-based flow system both exhibit eight to twenty-fold enhancement in catalysis efficiency compared to their batch counterparts, and a durability of at least 4000 h for the enantioselective trans-esterification of 1-phenylethyl alcohol, otherwise unattainable in their batch counterparts. We further establish a theoretical model for such a catalysis system working under non-equilibrium conditions, which not only supports the experimental results but also helps to predict reaction progress at a microscale level. Being operationally simple, efficient and adaptive, this strategy provides an unprecedented platform for practical applications of enzymes and homogeneous catalysts even at a controllable level.

Citation

Zhang, M., Ettelaie, R., Yan, T., Zhang, S., Cheng, F., Binks, B. P., & Yang, H. (2017). Ionic liquid droplet micro-reactor for catalysis reactions not at equilibrium. Journal of the American Chemical Society, 139(48), 17387-17396. https://doi.org/10.1021/jacs.7b07731

• Journal Article Type: Article
• Acceptance Date: Nov 3, 2017
• Online Publication Date: Nov 3, 2017
• Publication Date: Dec 6, 2017
• Deposit Date: Nov 13, 2017
• Publicly Available Date: Nov 5, 2018
• Journal: Journal of the American Chemical Society
• Print ISSN: 0002-7863
• Publisher: American Chemical Society
• Peer Reviewed: Peer Reviewed
• Volume: 139
• Issue: 48
• Pages: 17387-17396
• DOI: https://doi.org/10.1021/jacs.7b07731
• Keywords: Catalysis reactions
• Public URL: https://hull-repository.worktribe.com/output/456488
• Publisher URL: http://pubs.acs.org/doi/10.1021/jacs.7b07731
• Additional Information: This is the accepted manuscript of an article published in Journal of the American Chemical Society, 2017. The version of record is available at the DOI link in this record.
• Contract Date: Nov 13, 2017