TY - JOUR
T1 - The Porosity, Acidity, and Reactivity of Dealuminated Zeolite ZSM-5 at the Single Particle Level
T2 - The Influence of the Zeolite Architecture
AU - Aramburo, Luis R.
AU - Karwacki, Lukasz
AU - Cubillas, Pablo
AU - Asahina, Shunsuke
AU - de Winter, D. A. Matthijs
AU - Drury, Martyn R.
AU - Buurmans, Inge L. C.
AU - Stavitski, Eli
AU - Mores, Davide
AU - Daturi, Marco
AU - Bazin, Philippe
AU - Dumas, Paul
AU - Thibault-Starzyk, Frederic
AU - Post, Jan A.
AU - Anderson, Michael W.
AU - Terasaki, Osamu
AU - Weckhuysen, Bert M.
PY - 2011/12
Y1 - 2011/12
N2 - A combination of atomic force microscopy (AFM), high-resolution scanning electron microscopy (HR-SEM), focused-ion-beam scanning electron microscopy (FIB-SEM), X-ray photoelectron spectroscopy (XPS), confocal fluorescence microscopy (CFM), and UV/Vis and synchrotron-based IR microspectroscopy was used to investigate the dealumination processes of zeolite ZSM-5 at the individual crystal level. It was shown that steaming has a significant impact on the porosity, acidity, and reactivity of the zeolite materials. The catalytic performance, tested by the styrene oligomerization and methanol-to-olefin reactions, led to the conclusion that mild steaming conditions resulted in greatly enhanced acidity and reactivity of dealuminated zeolite ZSM-5. Interestingly, only residual surface mesoporosity was generated in the mildly steamed ZSM-5 zeolite, leading to rapid crystal coloration and coking upon catalytic testing and indicating an enhanced deactivation of the zeolites. In contrast, harsh steaming conditions generated 550 nm mesopores, extensively improving the accessibility of the zeolites. However, severe dealumination decreased the strength of the Bronsted acid sites, causing a depletion of the overall acidity, which resulted in a major drop in catalytic activity.
AB - A combination of atomic force microscopy (AFM), high-resolution scanning electron microscopy (HR-SEM), focused-ion-beam scanning electron microscopy (FIB-SEM), X-ray photoelectron spectroscopy (XPS), confocal fluorescence microscopy (CFM), and UV/Vis and synchrotron-based IR microspectroscopy was used to investigate the dealumination processes of zeolite ZSM-5 at the individual crystal level. It was shown that steaming has a significant impact on the porosity, acidity, and reactivity of the zeolite materials. The catalytic performance, tested by the styrene oligomerization and methanol-to-olefin reactions, led to the conclusion that mild steaming conditions resulted in greatly enhanced acidity and reactivity of dealuminated zeolite ZSM-5. Interestingly, only residual surface mesoporosity was generated in the mildly steamed ZSM-5 zeolite, leading to rapid crystal coloration and coking upon catalytic testing and indicating an enhanced deactivation of the zeolites. In contrast, harsh steaming conditions generated 550 nm mesopores, extensively improving the accessibility of the zeolites. However, severe dealumination decreased the strength of the Bronsted acid sites, causing a depletion of the overall acidity, which resulted in a major drop in catalytic activity.
KW - Acidity
KW - Dealumination
KW - Scanning probe microscopy
KW - Surface analysis
KW - Zeolites
UR - https://www.webofscience.com/api/gateway?GWVersion=2&SrcApp=d7dz6a2i7wiom976oc9ff2iqvdhv8k5x&SrcAuth=WosAPI&KeyUT=WOS:000298060800022&DestLinkType=FullRecord&DestApp=WOS
U2 - 10.1002/chem.201101361
DO - 10.1002/chem.201101361
M3 - Article
C2 - 22052456
SN - 0947-6539
VL - 17
SP - 13773
EP - 13781
JO - Chemistry-A European Journal
JF - Chemistry-A European Journal
IS - 49
ER -