Influence of active-site proximity in zeolites on Brønsted acid-catalyzed reactions at the microscopic and mesoscopic levels

Teng Li, Sang Ho Chung, Stefan Nastase, Adrian Galilea, Yan Wang, Ildar Mukhambetov, Moussa Zaarour, Juan Carlos Navarro de Miguel, Jurjen Cazemier, Abhay Dokania, Liliana Panarone, Jorge Gascon, Luigi Cavallo, Javier Ruiz-Martínez*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

10 Scopus citations

Abstract

Zeolites are the catalytic workhorses of various relevant reactions, primarily because of their acidic properties. However, there have been few studies on unraveling the influence of Al distribution on acid-catalyzed reactions at the mesoscopic and microscopic levels. Taking the methanol-to-aromatics (MTA) process as a paradigm, we compared the catalytic performance of two H-ZSM-5 zeolites with comparable properties, except for Al distribution, i.e., intraparticle distribution and Al proximity at the nanoscale. Our results demonstrate that Al enrichment at positions closer to the external surface results in more paired acid sites that exhibit enhanced activity than the isolated ones. Moreover, such Al organization accelerates progression of cascade reactions to yield aromatics and alleviate their diffusion out. Exploiting this Al-zoning feature, we further fabricated hollow zeolites by desilication. Combining the optimized active sites with the improved diffusion and void-confinement properties of hollow crystals results in the highest capacity to produce aromatics.

Original languageEnglish (US)
Article number100540
JournalChem Catalysis
Volume3
Issue number6
DOIs
StatePublished - Jun 15 2023

Keywords

  • Al zoning
  • aluminum distribution
  • hollow zeolite
  • isolated acid sites
  • methanol to aromatics
  • paired acid sites
  • SDG9: Industry innovation and infrastructure
  • zeolite

ASJC Scopus subject areas

  • Chemistry (miscellaneous)
  • Physical and Theoretical Chemistry
  • Organic Chemistry

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