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

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

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

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. [Figure not available: see fulltext.]

Original languageEnglish
Pages (from-to)921-931
Number of pages11
JournalNature Catalysis
Volume3
Issue number11
Early online date26 Oct 2020
DOIs
Publication statusPublished - 1 Nov 2020

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