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A Spatially Orthogonal Hierarchically Porous Acid-Base Catalyst for Cascade and Antagonistic Reactions

preprint
revised on 23.05.2020 and posted on 26.05.2020 by Mark Isaacs, christopher parlett, neil robinson, Lee Durndell, Jinesh Manayil, Simon Beaumont, Shan Jiang, Nicole Hondow, Alexander Lamb, Michael Johns, Karen Wilson, Adam Lee

Complex organic molecules are of great importance to academic and industrial chemistry and typically synthesised 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 functionalised with a sulfated zirconia solid acid coating, while the mesopores are selectively functionalised with MgO solid base nanoparticles. Active site compartmentalisation 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 deacetylation-Knoevenagel condensation of dimethyl acetals to cyanoates.

History

Email Address of Submitting Author

adam.lee2@rmit.edu.au

Institution

RMIT University

Country

Australia

ORCID For Submitting Author

0000-0002-2153-1391

Declaration of Conflict of Interest

The authors hereby declare that there are no conflicts of interest.

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