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Impact of Controlling the Site Distribution of Al Atoms on Catalytic Properties in Ferrierite-Type Zeolites

Román-Leshkov, Yuriy and Moliner, Manuel and Davis, Mark E. (2011) Impact of Controlling the Site Distribution of Al Atoms on Catalytic Properties in Ferrierite-Type Zeolites. Journal of Physical Chemistry C, 115 (4). pp. 1096-1102. ISSN 1932-7447. https://resolver.caltech.edu/CaltechAUTHORS:20110303-143355838

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Abstract

Zeolites with the ferrierite (FER) topology are synthesized using a combination of tetramethylammonium (TMA) cations with differently sized cyclic amines (pyrrolidine (Pyr), hexamethyleneimine (HMI), and 1,4- diazabicyclo[2.2.2]octane (DAB)). Using these organic structure-directing agents (SDAs), low Si/Al ratios and concentrated synthesis mixtures favor the crystallization of FER materials. Increasing the size of the cyclic amine or decreasing the aluminum content leads to the crystallization of other phases or the creation of excessive amounts of connectivity defects. TMA cations play a decisive role in the synthesis of the FER materials, and their presence allows the use of HMI to synthesize FER. Proton MAS NMR is used to quantify the accessibility of pyridine to acid sites in these FER samples, where it is found that the FER + HMI + TMA sample contains only 27% acid sites in the 8-MR channels, whereas FER + Pyr and FER + Pyr + TMA contain 89% and 84%, respectively. The constraint index (CI) test and the carbonylation of dimethyl ether (DME) with carbon monoxide are used as probe reactions to evaluate how changes in the aluminum distribution in these FER samples affect their catalytic behavior. Results show that the use of Pyr as an SDA results in the selective population of acid sites in the 8-MR channels, whereas the use of HMI generates FER zeolites with an increased concentration of acid sites in the 10-MR channels.


Item Type:Article
Related URLs:
URLURL TypeDescription
http://dx.doi.org/10.1021/jp106247gDOIArticle
ORCID:
AuthorORCID
Román-Leshkov, Yuriy0000-0002-0025-4233
Moliner, Manuel0000-0002-5440-716X
Davis, Mark E.0000-0001-8294-1477
Additional Information:© 2011 American Chemical Society. Received: July 6, 2010. Publication Date (Web): September 9, 2010. Part of the “Alfons Baiker Festschrift”. Financial support for the work was provided by British Petroleum. M.M. acknowledges the Fundaciόn Ramόn Areces Postdoctoral Research Fellowship Program for financial support.
Funders:
Funding AgencyGrant Number
British PetroleumUNSPECIFIED
Fundaciόn Ramόn Areces Postdoctoral Research Fellowship ProgramUNSPECIFIED
Issue or Number:4
Record Number:CaltechAUTHORS:20110303-143355838
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20110303-143355838
Official Citation:Impact of Controlling the Site Distribution of Al Atoms on Catalytic Properties in Ferrierite-Type Zeolites Yuriy Romn-Leshkov, Manuel Moliner, Mark E. Davis The Journal of Physical Chemistry C 2011 115 (4), 1096-1102
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:22643
Collection:CaltechAUTHORS
Deposited By: Ruth Sustaita
Deposited On:03 Mar 2011 23:03
Last Modified:03 Oct 2019 02:39

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