CHARACTERIZATION OF CATALYST ACIDITY BY MICROCALORIMETRY AND TEMPERATURE-PROGRAMMED DESORPTION

被引:99
|
作者
SHARMA, SB
MEYERS, BL
CHEN, DT
MILLER, J
DUMESIC, JA
机构
[1] UNIV WISCONSIN,DEPT CHEM ENGN,MADISON,WI 53706
[2] AMOCO RES CTR,NAPERVILLE,IL 60566
关键词
ACIDITY; AMMONIA; MICROCALORIMETRY; MORDENITE; TPD; ZSM-5;
D O I
10.1016/0926-860X(93)80232-F
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
Microcalorimetric measurements and temperature-programmed desorption (TPD) experiments were conducted to study the acidic properties of H-mordenite and H-ZSM-5. Both zeolites possess a relatively homogeneous acid-strength distribution. The enthalpy changes of adsorption for ammonia on H-mordenite and H-ZSM-5 are - 157 and - 150 kJ mol-1, respectively. Analyses of the TPD spectra, constrained by the microcalorimetric results, indicate that the standard entropy changes of ammonia adsorption on H-mordenite and H-ZSM-5 are - 159 and - 171 J mol-1 K-1, respectively. Accordingly, ammonia retains a significant fraction of its local entropy on H -mordenite (i.e., rotation and vibration), while ammonia adsorbed on H-ZSM-5 loses approximately a third of its local entropy. Pyridine desorption from these zeolites is limited by molecular diffusion in the zeolite particles and for this reason is a poor choice as a probe molecule for assessment of acid-site strength by TPD.
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页码:253 / 265
页数:13
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