Zeolite Synthesis in the Presence of Metallosiloxanes for the Quantitative Encapsulation of Metal Species for the Selective Catalytic Reduction (SCR) of NOx

Rushana Khairova, Sarah Komaty, Alla Dikhtiarenko, Jose Luis Cerrillo, Sudheesh Kumar Veeranmaril, Selvedin Telalović, Antonio Aguilar Tapia, Jean Louis Hazemann, Javier Ruiz-Martinez*, Jorge Gascon*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

3 Scopus citations

Abstract

Metal encapsulation in zeolitic materials through one-pot hydrothermal synthesis (HTS) is an attractive technique to prepare zeolites with a high metal dispersion. Due to its simplicity and the excellent catalytic performance observed for several catalytic systems, this method has gained a great deal of attention over the last few years. While most studies apply synthetic methods involving different organic ligands to stabilize the metal under synthesis conditions, here we report the use of metallosiloxanes as an alternative metal precursor. Metallosiloxanes can be synthesized from simple and cost-affordable chemicals and, when used in combination with zeolite building blocks under standard synthesis conditions, lead to quantitative metal loading and high dispersion. Thanks to the structural analogy of siloxane with TEOS, the synthesis gel stabilizes by forming siloxane bridges that prevent metal precipitation and clustering. When focusing on Fe-encapsulation, we demonstrate that Fe-MFI zeolites obtained by this method exhibit high catalytic activity in the NH3-mediated selective catalytic reduction (SCR) of NOx along with a good H2O/SO2 tolerance. This synthetic approach opens a new synthetic route for the encapsulation of transition metals within zeolite structures.

Original languageEnglish (US)
Article numbere202311048
JournalAngewandte Chemie - International Edition
Volume62
Issue number40
DOIs
StatePublished - Oct 2 2023

Bibliographical note

Funding Information:
Funding for this work was provided by King Abdullah University of Science and Technology (KAUST). The authors gratefully thank Dr. Nimer Wehbe and Dr. Qingxiao Wang from Imaging and Characterization Department Core Labs for X‐ray Photoelectron Spectroscopy (XPS) and Transmission electron microscopy (TEM) measurements and discussion. We acknowledge the European Synchrotron Radiation Facility for provision of synchrotron radiation facilities, and we would like to thank Eric Lahera for assistance in using beamline BM30.

Publisher Copyright:
© 2023 Wiley-VCH GmbH.

Keywords

  • HO/SO Tolerance
  • Iron
  • Selective Catalytic Reduction (SCR)
  • Single-Site Catalyst
  • Zeolite

ASJC Scopus subject areas

  • Catalysis
  • General Chemistry

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