ArticleJournal of the American Chemical Society2021
Design and Synthesis of the Active Site Environment in Zeolite Catalysts for Selectively Manipulating Mechanistic Pathways.
Article in Journal of the American Chemical Society, 2021. 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.
- In Situ NMR and Kinetics Reveal Origins of Regioselectivity Differences for Epichlorohydrin Ring-Opening in Lewis and Brønsted Acid Zeolites.Angewandte Chemie (International ed. in English) · 2025Article
- Screening Cu-Zeolites for Methane Activation Using Curriculum-Based Training.ACS catalysis · 2024Article
- Approaching enzymatic catalysis with zeolites or how to select one reaction mechanism competing with others.Nature communications · 2023Article
- Impact of a polymer modifier on directing the non-classical crystallization pathway of TS-1 zeolite: accelerating nucleation and enriching active sites.Chemical science · 2022Article
- Switching between classical/nonclassical crystallization pathways of TS-1 zeolite: implication on titanium distribution and catalysis.Chemical science · 2022Article
- Enhanced C-H bond activation by tuning the local environment of surface lattice oxygen of MoOChemical science · 2022Article
- Mechanistic Characterization of Zeolite-Catalyzed Aromatic Electrophilic Substitution at Realistic Operating Conditions.JACS Au · 2022Article
Corrections and comments
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Authors and funding
6 authors.
Funding
No grant is acknowledged in the PubMed record.
Abstract
By combining kinetics and theoretical calculations, we show here the benefits of going beyond the concept of static localized and defined active sites on solid catalysts, into a system that globally and dynamically considers the active site located in an environment that involves a scaffold structure particularly suited for a target reaction. We demonstrate that such a system is able to direct the reaction through a preferred mechanism when two of them are competing. This is illustrated here for an industrially relevant reaction, the diethylbenzene-benzene transalkylation. The zeolite catalyst (ITQ-27) optimizes location, density, and environment of acid sites to drive the reaction through the preselected and preferred diaryl-mediated mechanism, instead of the alkyl transfer pathway. This is achieved by minimizing the activation energy of the selected pathway through weak interactions, much in the way that it occurs in enzymatic catalysts. We show that ITQ-27 outperforms previously reported zeolites for the DEB-Bz transalkylation and, more specifically, industrially relevant zeolites such as faujasite, beta, and mordenite.
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Registered trials
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