ArticleJournal of the American Chemical Society2024
Origins of High-Activity Cage-Catalyzed Michael Addition.
Article in Journal of the American Chemical Society, 2024. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Cited by 7 papers.
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Who cites it
7 citing papers in PubMed.
- Mechanochemical disassembly pathways of self-assembled polymer-decorated PdNature communications · 2026Article
- Selective photocatalytic oxidative cleavage of terminal alkynes to carboxylic acids within a water-soluble PdChemical science · 2026Article
- Attractive Noncovalent Interactions versus Steric Confinement in Asymmetric Supramolecular Catalysis.Journal of the American Chemical Society · 2026Article
- Formation of a PdJACS Au · 2025Article
- Dissecting the Effects of Cage Structure in the Catalytic Activation of Imide Chlorenium-Ion Donors.Journal of the American Chemical Society · 2025Article
- Beyond symmetric self-assembly and effective molarity: unlocking functional enzyme mimics with robust organic cages.Beilstein journal of organic chemistry · 2025Article
- Photoswitchable Catalysis by a Self-Assembled Molecular Cage.Journal of the American Chemical Society · 2024Article
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Authors and funding
7 authors.
Funding
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Abstract
Cage catalysis continues to create significant interest, yet catalyst function remains poorly understood. Herein, we report mechanistic insights into coordination-cage-catalyzed Michael addition using kinetic and computational methods. The study has been enabled by the detection of identifiable catalyst intermediates, which allow the evolution of different cage species to be monitored and modeled alongside reactants and products. The investigations show that the overall acceleration results from two distinct effects. First, the cage reaction shows a thousand-fold increase in the rate constant for the turnover-limiting C-C bond-forming step compared to a reference state. Computational modeling and experimental analysis of activation parameters indicate that this stems from a significant reduction in entropy, suggesting substrate coencapsulation. Second, the cage markedly acidifies the bound pronucleophile, shifting this equilibrium by up to 6 orders of magnitude. The combination of these two factors results in accelerations up to 10
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Registered trials
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