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.

doi:10.1038/s41929-020-00526-5

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.

Authors

Mark A. Isaacs

Christopher M.A. Parlett

Neil Robinson

Lee J. Durndell

Jinesh C. Manayil

Dr Simon Beaumont simon.beaumont@durham.ac.uk
Associate Professor

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., Jiang, S., Hondow, N. S., Lamb, A. C., Jampaiah, D., Johns, M. L., Wilson, 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
Public URL	https://durham-repository.worktribe.com/output/1256885