Zhang, X, Hou, Y, Ettelaie, R orcid.org/0000-0002-6970-4650 et al. (4 more authors) (2019) Pickering Emulsion-Derived Liquid–Solid Hybrid Catalyst for Bridging Homogeneous and Heterogeneous Catalysis. Journal of the American Chemical Society, 141 (13). pp. 5220-5230. ISSN 0002-7863
Abstract
We describe a novel method to prepare a liquid-solid hybrid catalyst via interfacial growth of a porous silica crust around Pickering emulsion droplets, which allowed us to overcome the current limitations of both homogeneous and heterogeneous catalysts. The inner micron-scaled liquid (for example, ionic liquids) pool of the resultant catalyst can host free homogeneous molecular catalysts or enzymes to create a true homogeneous catalysis environment. The porous silica crust of the hybrid catalyst has excellent stability, which makes it amenable to packing directly in fixed-bed reactors for continuous flow catalysis. As a proof of concept, the enzymatic kinetic resolution of racemic alcohols, CrIII(salen) complex-catalyzed asymmetric ring opening of epoxides and Pd-catalyzed Tsuji-Trost allylic substitution reactions were used to verify the generality and versatility of our strategy for bridging homogeneous and heterogeneous catalysis. The hybrid catalyst-based continuous flow system exhibited a 1.6~16-fold enhancement in activity relative to homogeneous counterparts even at more than 1500 h, and the afforded enantioselectivities were completely equal to those obtained in the homogeneous counterpart systems. Interestingly, the catalytic efficiency can be tuned through rational engineering of the porous crust and the dimensions of the liquid pool, resulting in features of an innovatively designed catalyst. This contribution provides a new method to design efficient catalysts that can bridge the conceptual and technical gaps between homogeneous and heterogeneous catalysis.
Metadata
Item Type: | Article |
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Authors/Creators: |
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Copyright, Publisher and Additional Information: | (c) 2019, American Chemical Society. This is an author produced version of a paper published in Journal of the American Chemical Society . Uploaded in accordance with the publisher's self-archiving policy. |
Keywords: | Homogeneous and Heterogeneous Catalysis; Pickering emulsions; Ioinc liquids |
Dates: |
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Institution: | The University of Leeds |
Academic Units: | The University of Leeds > Faculty of Environment (Leeds) > School of Food Science and Nutrition (Leeds) > FSN Colloids and Food Processing (Leeds) |
Depositing User: | Symplectic Publications |
Date Deposited: | 21 Feb 2019 09:13 |
Last Modified: | 01 Feb 2021 15:36 |
Status: | Published |
Publisher: | American Chemical Society |
Identification Number: | 10.1021/jacs.8b11860 |
Open Archives Initiative ID (OAI ID): | oai:eprints.whiterose.ac.uk:142777 |