INTERCAGE AND INTRACAGE TRANSPORT OF AROMATICS IN ZEOLITES NAY, HY, AND USY STUDIED BY H-2 NMR

被引:36
作者
GONCALVES, JAS
PORTSMOUTH, RL
ALEXANDER, P
GLADDEN, LF
机构
[1] UNIV CAMBRIDGE,DEPT CHEM ENGN,CAMBRIDGE CB2 3RA,ENGLAND
[2] UNIV CAMBRIDGE,DEPT PHYS,CAMBRIDGE CB3 0HE,ENGLAND
关键词
D O I
10.1021/j100010a049
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
Adsorption and transport characteristics of benzene and p-xylene in three forms of zeolite Y are reported: NaY (Si/Al = 2.65), HY (Si/Al = 3.25), and USY (Si/Al 40). H-2 NMR line-shape studies and both independent and simultaneous analysis of the temperature-dependence of spin-lattice and spin-spin relaxation times of the deuterated sorbates confined within the zeolite frameworks are compared as methods of characterizing sorption phenomena and estimating diffusion coefficients and activation energies to site-hopping motions within the zeolite framework. Both benzene and p-xylene in NaY show evidence of one site-hopping motion characterized by an activation energy of 25.8 and 32.0 kJ mol(-1), respectively. In contrast the same sorbates confined within HY and USY show two different motional regimes. Below 260 K, activation energies on the order of 10-15 kJ mol(-1) are measured, whereas above this temperature larger activation energies of 24-30 kJ mol(-1) are typical. It is suggested that the higher activation energies are associated with intercage jump processes, while the lower activation energies are characteristic of intracage transport. The lack of a low-energy activated translational process in NaY suggests that the sorbed aromatics are tightly bound to the Na+ occurring increases with increase in Si/Al ratio, decrease in sorbate concentration, and decrease in the size of the exchangeable cation.
引用
收藏
页码:3317 / 3325
页数:9
相关论文
共 28 条
[1]  
Barrer R.M., 1978, ZEOLITES CLAY MINERA
[2]   PROTON AND DEUTERON MAGNETIC-RESONANCE RELAXATION OF BENZENE ADSORBED ON ALUMINA AND ON A PLATINUM ALUMINA CATALYST [J].
BODDENBERG, B ;
BEERWERTH, B .
JOURNAL OF PHYSICAL CHEMISTRY, 1989, 93 (04) :1440-1447
[3]   H-2 NMR-STUDY ON THE ROTATION AND DIFFUSION KINETICS OF PROPENE AND BENZENE IN NAX AND AGNAX ZEOLITES [J].
BODDENBERG, B ;
BURMEISTER, R .
ZEOLITES, 1988, 8 (06) :488-494
[4]  
BRECK DW, 1984, ZEOLITE MOL SIEVES
[5]   BEHAVIOR OF BENZENE IN SILICEOUS FAUJASITE - A COMPARATIVE-STUDY BY H-2 NMR AND MOLECULAR-DYNAMICS [J].
BULL, LM ;
HENSON, NJ ;
CHEETHAM, AK ;
NEWSAM, JM ;
HEYES, SJ .
JOURNAL OF PHYSICAL CHEMISTRY, 1993, 97 (45) :11776-11780
[6]  
BULL LM, 1993, 9TH P INT ZEOL C MON, P63
[7]   INTRACRYSTALLINE DIFFUSION OF BENZENE IN NAX ZEOLITE STUDIED BY SORPTION KINETICS [J].
BULOW, M ;
MIETK, W ;
STRUVE, P ;
LORENZ, P .
JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS I, 1983, 79 :2457-2466
[8]   THE DETERMINATION OF TRANSLATIONAL INTRACRYSTALLINE DIFFUSION CONSTANTS OF MOLECULES IN FAUJASITE-TYPE ZEOLITES WITH THE AID OF DEUTERON-NMR-SPECTROSCOPY [J].
BURMEISTER, R ;
SCHWARZ, H ;
BODDENBERG, B .
BERICHTE DER BUNSEN-GESELLSCHAFT-PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 1989, 93 (11) :1309-1313
[9]  
CASCI JL, COMMUNICATION
[10]   LOCALIZATION AND MOBILITY OF BENZENE IN SODIUM-Y ZEOLITE BY MOLECULAR-DYNAMICS CALCULATIONS [J].
DEMONTIS, P ;
YASHONATH, S ;
KLEIN, ML .
JOURNAL OF PHYSICAL CHEMISTRY, 1989, 93 (13) :5016-5019