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