Water-Induced Micro-Hydrophobic Effect Regulates Benzene Methylation in Zeolite.
Angew Chem Int Ed Engl
; 63(3): e202313974, 2024 Jan 15.
Article
em En
| MEDLINE
| ID: mdl-37934010
ABSTRACT
Water is a ubiquitous component in heterogeneous catalysis over zeolites and can significantly influence the catalyst performance. However, the detailed mechanism insights into zeolite-catalyzed reactions under microscale aqueous environment remain elusive. Here, using multiple dimensional solid-state NMR experiments coupled with ultrahigh magic angle spinning technique and theoretical simulations, we establish a fundamental understanding of the role of water in benzene methylation over ZSM-5 zeolite under water vapor conditions. We show that water competes with benzene for the active sites of zeolite and facilitates the bimolecular reaction mechanism. The growth of water clusters induces a micro-hydrophobic effect in zeolite pores, which reorients benzene molecules and drives their interactions with surface methoxy species (SMS) on zeolite. We identify the formation and evolution of active SMS-Benzene complexes in a microscale aqueous environment and demonstrate that their accumulation in zeolite pores boosts benzene conversion and methylation.
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Coleções:
01-internacional
Base de dados:
MEDLINE
Idioma:
En
Ano de publicação:
2024
Tipo de documento:
Article