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A spatially orthogonal hierarchically porous acid–base catalyst for cascade and antagonistic reactions

Isaacs, Mark A.; Parlett, Christopher M.A.; Robinson, Neil; Durndell, Lee J.; Manayil, Jinesh C.; Beaumont, Simon K.; Jiang, Shan; Hondow, Nicole S.; Lamb, Alexander C.; Jampaiah, Deshetti; Johns, Michael L.; Wilson, Karen; Lee, Adam F.

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Authors

Mark A. Isaacs

Christopher M.A. Parlett

Neil Robinson

Lee J. Durndell

Jinesh C. Manayil

Shan Jiang

Nicole S. Hondow

Alexander C. Lamb

Deshetti Jampaiah

Michael L. Johns

Karen Wilson

Adam F. Lee



Abstract

Complex organic molecules are of great importance to research and industrial chemistry and typically synthesized from smaller building blocks by multistep reactions. The ability to perform multiple (distinct) transformations in a single reactor would greatly reduce the number of manipulations required for chemical manufacturing, and hence the development of multifunctional catalysts for such one-pot reactions is highly desirable. Here we report the synthesis of a hierarchically porous framework, in which the macropores are selectively functionalized with a sulfated zirconia solid acid coating, while the mesopores are selectively functionalized with MgO solid base nanoparticles. Active site compartmentalization and substrate channelling protects base-catalysed triacylglyceride transesterification from poisoning by free fatty acid impurities (even at 50 mol%), and promotes the efficient two-step cascade deacetalization-Knoevenagel condensation of dimethyl acetals to cyanoates.

Citation

Isaacs, M. A., Parlett, C. M., Robinson, N., Durndell, L. J., Manayil, J. C., Beaumont, S. K., …Lee, A. F. (2020). A spatially orthogonal hierarchically porous acid–base catalyst for cascade and antagonistic reactions. Nature Catalysis, 3(11), 921-931. https://doi.org/10.1038/s41929-020-00526-5

Journal Article Type Article
Online Publication Date Oct 26, 2020
Publication Date 2020
Deposit Date Nov 19, 2020
Publicly Available Date Apr 26, 2021
Journal Nature Catalysis
Publisher Nature Research
Peer Reviewed Peer Reviewed
Volume 3
Issue 11
Pages 921-931
DOI https://doi.org/10.1038/s41929-020-00526-5

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