Approaching Enzymatic Catalysis with Zeolites or How to Select One Reaction Mechanism Competing with Others

Overview

Journal Nat Commun

Specialty Biology

Date 2023 May 19

PMID 37208318

Authors

Pau Ferri

Chengeng Li

Daniel Schwalbe-Koda

Mingrou Xie

Manuel Moliner

Rafael Gomez-Bombarelli

Mercedes Boronat

Avelino Corma

Affiliations

Soon will be listed here.

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.

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