Detection of active sites for paraffin cracking on USY zeolite by 27Al MQMAS NMR operated at high magnetic field 16 T

被引:44
作者
Katada, N
Nakata, S
Kato, S
Kanehashi, K
Saito, K
Niwa, M
机构
[1] Tottori Univ, Fac Engn, Dept Mat Sci, Tottori 6808552, Japan
[2] Japan Sci & Technol Agcy, PRESTo, Convers & Control Adv Chem, Kawaguchi, Saitama 3320012, Japan
[3] Akita Univ, Fac Engn & Resource Sci, Dept Mat Proc Engn & Appl Chem Environm, Akita 0108502, Japan
[4] Nippon Steel Corp Ltd, Adv Technol Res Lab, Chiba 2938511, Japan
关键词
EDTA-treated USY zeolite; Al-27 3QMAS NMR; extra-framework Al; paraffin cracking; Bronsted acidity;
D O I
10.1016/j.molcata.2005.04.024
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
Al-27 MAS (magic angle spinning) and 3Q (triple quantum) MAS NMR (nuclear magnetic resonance) at a very high magnetic field (16 T, 700 MHz for H-1) enabled us to detect all the Al species on a series of modified Y zeolites. In a USY (ultra stable Y) zeolite after steaming, extra-framework Al species with various environments were detected, while only framework Al (IV) was observed in the parent NaY zeolite. 3QMAS NMR clearly identified the tetra-coordinated extra-framework Al with a large structural anisotropy (IVb), in addition to the penta-(V) and hexa-coordinated (VI) species. Na2H2-EDTA (ethylenediaminetetraacetic acid) treatment of the USY was found to convert the V and VI species into the IVb species. Increase in the Bronsted acid strength and the catalytic activity for octane cracking has been found on the Na2H2-EDTA-treated USY. Therefore, it is speculated that the IVb species is the origin of enhanced Bronsted acidity (and thereby the high cracking activity) of the USY zeolite. (c) 2005 Elsevier B.V. All rights reserved.
引用
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页码:239 / 245
页数:7
相关论文
共 19 条
[11]   Effect of steam dealumination on H-Y acidity and 2-methylpentane cracking activity [J].
Kuehne, MA ;
Kung, HH ;
Miller, JT .
JOURNAL OF CATALYSIS, 1997, 171 (01) :293-304
[12]   Structural evolution of dealuminated Y zeolites during KOH solution treatment [J].
Liu, DS ;
Bao, SL ;
Xu, QH .
ZEOLITES, 1997, 18 (2-3) :162-170
[13]   QUANTITATIVE-DETERMINATION OF ALUMINUM IN ZEOLITES BY SOLID-STATE AL-27 NMR-SPECTROSCOPY [J].
MAN, PP ;
KLINOWSKI, J .
JOURNAL OF THE CHEMICAL SOCIETY-CHEMICAL COMMUNICATIONS, 1988, (19) :1291-1294
[14]   Two-dimensional magic-angle spinning isotropic reconstruction sequences for quadrupolar nuclei [J].
Massiot, D ;
Touzo, B ;
Trumeau, D ;
Coutures, JP ;
Virlet, J ;
Florian, P ;
Grandinetti, PJ .
SOLID STATE NUCLEAR MAGNETIC RESONANCE, 1996, 6 (01) :73-83
[15]  
MCDANIEL CV, 1966, Patent No. 3292192
[16]  
Niwa M., 1997, CATAL SURV JPN, V1, P215, DOI [10.1023/A:1019033115091, DOI 10.1023/A:1019033115091, 10.1023/a:1019033115091]
[17]   PREDICTION OF CRACKING CATALYST BEHAVIOR BY A ZEOLITE UNIT-CELL SIZE MODEL [J].
PINE, LA ;
MAHER, PJ ;
WACHTER, WA .
JOURNAL OF CATALYSIS, 1984, 85 (02) :466-476
[18]   Dealuminated H-Y zeolites: Relation between physicochemical properties and catalytic activity in heptane and decane isomerization [J].
Remy, MJ ;
Stanica, D ;
Poncelet, G ;
Feijen, EJP ;
Grobet, PJ ;
Martens, JA ;
Jacobs, PA .
JOURNAL OF PHYSICAL CHEMISTRY, 1996, 100 (30) :12440-12447
[19]  
Suzuki K., UNPUB