Approaching enzymatic catalysis with zeolites or how to select one reaction mechanism competing with others

Pau Ferri, Chengeng Li, Daniel Schwalbe-Koda, Mingrou Xie, Manuel Moliner, Rafael Gómez-Bombarelli, Mercedes Boronat () and Avelino Corma ()
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Pau Ferri: Universitat Politècnica de València - Consejo Superior de Investigaciones Científicas
Chengeng Li: Universitat Politècnica de València - Consejo Superior de Investigaciones Científicas
Daniel Schwalbe-Koda: Massachusetts Institute of Technology
Mingrou Xie: Massachusetts Institute of Technology
Manuel Moliner: Universitat Politècnica de València - Consejo Superior de Investigaciones Científicas
Rafael Gómez-Bombarelli: Massachusetts Institute of Technology
Mercedes Boronat: Universitat Politècnica de València - Consejo Superior de Investigaciones Científicas
Avelino Corma: Universitat Politècnica de València - Consejo Superior de Investigaciones Científicas

Nature Communications, 2023, vol. 14, issue 1, 1-13

Abstract: Abstract Approaching the level of molecular recognition of enzymes with solid catalysts is a challenging goal, achieved in this work for the competing transalkylation and disproportionation of diethylbenzene catalyzed by acid zeolites. The key diaryl intermediates for the two competing reactions only differ in the number of ethyl substituents in the aromatic rings, and therefore finding a selective zeolite able to recognize this subtle difference requires an accurate balance of the stabilization of reaction intermediates and transition states inside the zeolite microporous voids. In this work we present a computational methodology that, by combining a fast high-throughput screeening of all zeolite structures able to stabilize the key intermediates with a more computationally demanding mechanistic study only on the most promising candidates, guides the selection of the zeolite structures to be synthesized. The methodology presented is validated experimentally and allows to go beyond the conventional criteria of zeolite shape-selectivity.

Date: 2023
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DOI: 10.1038/s41467-023-38544-z

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