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

Isaacs, MA; Parlett, CMA; Robinson, N; Durndell, LJ; Manayil, JC; Beaumont, SK; Jiang, S; ... Lee, AF; + view all (2020) A spatially orthogonal hierarchically porous acid-base catalyst for cascade and antagonistic reactions. Nature Catalysis , 3 (11) pp. 921-931. 10.1038/s41929-020-00526-5. Green open access

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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.

Type: Article
Title: A spatially orthogonal hierarchically porous acid-base catalyst for cascade and antagonistic reactions
Open access status: An open access version is available from UCL Discovery
DOI: 10.1038/s41929-020-00526-5
Publisher version: https://doi.org/10.1038/s41929-020-00526-5
Language: English
Additional information: This version is the author accepted manuscript. For information on re-use, please refer to the publisher’s terms and conditions.
UCL classification: UCL
UCL > Provost and Vice Provost Offices > UCL BEAMS
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry
URI: https://discovery.ucl.ac.uk/id/eprint/10132413
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