Creation of Bronsted Acidity by Grafting Aluminum Isopropoxide on Silica under Controlled Conditions: Determination of the Number of Bronsted Sites and their Turnover Frequency for m-Xylene Isomerization

被引:25
作者
Caillot, Maxime [1 ,2 ]
Chaumonnot, Alexandra [2 ]
Digne, Mathieu [2 ]
Van Bokhoven, Jeroen A. [1 ,3 ]
机构
[1] ETH, CH-8093 Zurich, Switzerland
[2] IFP Energies Nouvelles, Direct Catalyse & Separat, F-69360 Solaize, France
[3] Paul Scherrer Inst, Lab Catalysis & Sustainable Chem LSK, CH-5232 Villigen, Switzerland
关键词
acidity; coverage degree; ethanol; silicates; thermogravimetry; ETHANOL DEHYDRATION; CATALYTIC-ACTIVITY; SURFACE-ACIDITY; CO ADSORPTION; ZEOLITES; MCM-41; H-ZSM-5; FTIR; IR; AL;
D O I
10.1002/cctc.201300824
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
There is not a unique BrOnsted acid site for aluminosilicates (ASAs). IR spectroscopy following CO adsorption proves the creation of BrOnsted acid sites on Al/SiO2 ASAs, which are synthesized by the deposition of aluminum species on hydroxylated silica. These sites are active for ethanol dehydration and m-xylene isomerization. Controlled deposition under anhydrous conditions optimizes the number of sites, whereas the presence of water leads to alumina agglomerates with no BrOnsted acidity. The turnover frequency for m-xylene isomerization (4.3x10(-4)s(-1)site(-1) at 350 degrees C, atmospheric pressure, and 0.6cm(3)h(-1) of m-xylene) is approximately 3times lower than that of the BrOnsted acid sites of Si/Al2O3 and 75times lower than that of an ultrastable Y-type zeolite without extra-framework aluminum.
引用
收藏
页码:832 / 841
页数:10
相关论文
共 39 条
[1]   Catalytic transformation of methyl benzenes over zeolite catalysts [J].
Al-Khattaf, S. ;
Akhtar, M. N. ;
Odedairo, T. ;
Aitani, A. ;
Tukur, N. M. ;
Kubu, M. ;
Musilova-Pavlackova, Z. ;
Cejka, J. .
APPLIED CATALYSIS A-GENERAL, 2011, 394 (1-2) :176-190
[2]  
[Anonymous], 2009, ANGEW CHEM INT ED, V48, P2891
[3]   Acid sites investigation of simple and mixed oxides by TPD and microcalorimetric techniques [J].
Auroux, A ;
Monaci, R ;
Rombi, E ;
Solinas, V ;
Sorrentino, A ;
Santacesaria, E .
THERMOCHIMICA ACTA, 2001, 379 (1-2) :227-231
[4]   Decomposition and aromatization of ethanol on ZSM-based catalysts [J].
Barthos, R. ;
Szechenyi, A. ;
Solymosi, F. .
JOURNAL OF PHYSICAL CHEMISTRY B, 2006, 110 (43) :21816-21825
[5]   INFRARED SPECTROSCOPIC OBSERVATIONS OF SURFACE BONDING IN PHYSICAL ADSORPTION - THE PHYSICAL ADSORPTION OF CO ON SIO2 SURFACES [J].
BEEBE, TP ;
GELIN, P ;
YATES, JT .
SURFACE SCIENCE, 1984, 148 (2-3) :526-550
[6]   Synthesis of amorphous aluminosilicates by grafting: Tuning the building and final structure of the deposit by selecting the appropriate synthesis conditions [J].
Caillot, Maxime ;
Chaumonnot, Alexandra ;
Digne, Mathieu ;
Poleunis, Claude ;
Debecker, Damien P. ;
van Bokhoven, Jeroen A. .
MICROPOROUS AND MESOPOROUS MATERIALS, 2014, 185 :179-189
[7]   Quantification of Bronsted Acid Sites of Grafted Amorphous Silica-Alumina Compounds and their Turnover Frequency in m-Xylene Isomerization [J].
Caillot, Maxime ;
Chaumonnot, Alexandra ;
Digne, Mathieu ;
Van Bokhoven, Jeroen A. .
CHEMCATCHEM, 2013, 5 (12) :3644-3656
[8]   Bronsted acidity of extraframework debris in steamed Y zeolites from the FTIR study of CO adsorption [J].
Cairon, O ;
Chevreau, T ;
Lavalley, JC .
JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS, 1998, 94 (19) :3039-3047
[9]   Large heterogeneity of Bronsted acid sites in ASA and USY zeolites: evidencing a third acidic component [J].
Cairon, Olivier .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2010, 12 (24) :6333-6336
[10]  
Chaumonnot A, 2013, IFP ENERG NOUV PUBL, P225