The Porosity, Acidity, and Reactivity of Dealuminated Zeolite ZSM-5 at the Single Particle Level: The Influence of the Zeolite Architecture

被引:95
作者
Aramburo, Luis R. [1 ]
Karwacki, Lukasz [1 ]
Cubillas, Pablo [2 ]
Asahina, Shunsuke [3 ,4 ]
de Winter, D. A. Matthijs [5 ]
Drury, Martyn R. [6 ]
Buurmans, Inge L. C. [1 ]
Stavitski, Eli [1 ]
Mores, Davide [1 ]
Daturi, Marco [7 ]
Bazin, Philippe [7 ]
Dumas, Paul [8 ]
Thibault-Starzyk, Frederic [7 ]
Post, Jan A. [5 ]
Anderson, Michael W. [2 ]
Terasaki, Osamu [9 ,10 ]
Weckhuysen, Bert M. [1 ]
机构
[1] Univ Utrecht, Debye Inst NanoMat Sci, NL-3584 CG Utrecht, Netherlands
[2] Univ Manchester, Ctr Nanoporous Mat, Sch Chem, Manchester M13 9LP, Lancs, England
[3] JEOL Europe SAS Espace Claude Monet, European Applicat Grp, F-78290 Allbe De Givemy, Croissy Sur Sei, France
[4] Tohoku Univ, Inst Multidisciplinary Res Adv Mat, Sendai, Miyagi 9808577, Japan
[5] Univ Utrecht, Fac Sci, NL-3584 CH Utrecht, Netherlands
[6] Univ Utrecht, Dept Earth Sci, Fac Geosci, NL-3508 TA Utrecht, Netherlands
[7] Lab Catalyse & Spectrochim, F-14050 Caen, France
[8] Synchrotron SOLEIL, Gif Sur Yvette, France
[9] Korea Adv Inst Sci & Technol, Grad Sch EEWS WCU, Taejon 305701, South Korea
[10] Stockholm Univ, Dept Mat & Environm Chem, S-10691 Stockholm, Sweden
关键词
acidity; dealumination; scanning probe microscopy; surface analysis; zeolites; ATOMIC-FORCE MICROSCOPY; MOLECULAR-DIFFUSION; CATALYTIC-ACTIVITY; H-ZSM-5; CRYSTALS; CONVERSION; MICROSPECTROSCOPY; HYDROCARBON; BARRIERS; METHANOL; CRACKING;
D O I
10.1002/chem.201101361
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
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.
引用
收藏
页码:13773 / 13781
页数:9
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