TY - JOUR
T1 - Disentangling Reaction Processes of Zeolites within Single-Oriented Channels
AU - Fu, Donglong
AU - van der Heijden, Onno
AU - Stanciakova, Katarina
AU - Schmidt, Joel E
AU - Weckhuysen, Bert M
N1 - © 2020 The Authors. Published by Wiley-VCH Verlag GmbH & Co. KGaA.
PY - 2020/9/1
Y1 - 2020/9/1
N2 - Establishing structure-reactivity relationships for specific channel orientations of zeolites is vital to developing new, superior materials for various applications, including oil and gas conversion processes. Herein, a well-defined model system was developed to build structure-reactivity relationships for specific zeolite-channel orientations during various catalytic reaction processes, for example, the methanol- and ethanol-to-hydrocarbons (MTH and ETH) process as well as oligomerization reactions. The entrapped and effluent hydrocarbons from single-oriented zeolite ZSM-5 channels during the MTH process were monitored by using operando UV/Vis diffuse reflectance spectroscopy (DRS) and on-line mass spectrometry (MS), respectively. The results reveal that the straight channels favor the formation of internal coke, promoting the aromatic cycle. Furthermore, the sinusoidal channels produce aromatics, (e.g., toluene) that further grow into larger polyaromatics (e.g., graphitic coke) leading to deactivation of the zeolites. This underscores the importance of careful engineering of materials to suppress coke formation and tune product distribution by rational control of the location of zeolite acid sites and crystallographic orientations.
AB - Establishing structure-reactivity relationships for specific channel orientations of zeolites is vital to developing new, superior materials for various applications, including oil and gas conversion processes. Herein, a well-defined model system was developed to build structure-reactivity relationships for specific zeolite-channel orientations during various catalytic reaction processes, for example, the methanol- and ethanol-to-hydrocarbons (MTH and ETH) process as well as oligomerization reactions. The entrapped and effluent hydrocarbons from single-oriented zeolite ZSM-5 channels during the MTH process were monitored by using operando UV/Vis diffuse reflectance spectroscopy (DRS) and on-line mass spectrometry (MS), respectively. The results reveal that the straight channels favor the formation of internal coke, promoting the aromatic cycle. Furthermore, the sinusoidal channels produce aromatics, (e.g., toluene) that further grow into larger polyaromatics (e.g., graphitic coke) leading to deactivation of the zeolites. This underscores the importance of careful engineering of materials to suppress coke formation and tune product distribution by rational control of the location of zeolite acid sites and crystallographic orientations.
KW - methanol conversion
KW - structure–reactivity relationships
KW - thin films
KW - zeolites
KW - ZSM-5
U2 - 10.1002/anie.201916596
DO - 10.1002/anie.201916596
M3 - Article
C2 - 32026555
SN - 1433-7851
VL - 59
SP - 15502
EP - 15506
JO - Angewandte Chemie-International Edition
JF - Angewandte Chemie-International Edition
IS - 36
ER -