TY - JOUR
T1 - Zeolite Synthesis in the Presence of Metallosiloxanes for the Quantitative Encapsulation of Metal Species for the Selective Catalytic Reduction (SCR) of NOx
AU - Khairova, Rushana
AU - Komaty, Sarah
AU - Dikhtiarenko, Alla
AU - Cerrillo, Jose Luis
AU - Veeranmaril, Sudheesh Kumar
AU - Telalović, Selvedin
AU - Tapia, Antonio Aguilar
AU - Hazemann, Jean Louis
AU - Ruiz-Martinez, Javier
AU - Gascon, Jorge
N1 - 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.
PY - 2023/10/2
Y1 - 2023/10/2
N2 - 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.
AB - 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.
KW - HO/SO Tolerance
KW - Iron
KW - Selective Catalytic Reduction (SCR)
KW - Single-Site Catalyst
KW - Zeolite
UR - http://www.scopus.com/inward/record.url?scp=85168861893&partnerID=8YFLogxK
U2 - 10.1002/anie.202311048
DO - 10.1002/anie.202311048
M3 - Article
C2 - 37581296
AN - SCOPUS:85168861893
SN - 1433-7851
VL - 62
JO - Angewandte Chemie - International Edition
JF - Angewandte Chemie - International Edition
IS - 40
M1 - e202311048
ER -