COMPARISON OF THE ACIDIC PROPERTIES OF H-[AL]ZSM-5, H-[FE]ZSM-5, AND H-[GA]ZSM-5 USING MICROCALORIMETRY, HEXANE CRACKING, AND PROPENE OLIGOMERIZATION

被引:75
作者
PARRILLO, DJ
LEE, C
GORTE, RJ
WHITE, D
FARNETH, WE
机构
[1] UNIV PENN,DEPT CHEM ENGN,PHILADELPHIA,PA 19104
[2] UNIV PENN,DEPT CHEM,PHILADELPHIA,PA 19104
[3] DUPONT CO INC,DEPT CENT SCI & ENGN,EXPTL STN,WILMINGTON,DE 19880
关键词
D O I
10.1021/j100021a046
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
We have used a combination of microcalorimetry measurements of ammonia and pyridine and reactivity measurements for n-hexane cracking, propene oligomerization, and 2-methyl-2-propanol decomposition to compare the acid sites in H-[Fe]ZSM-5, H-[Ga]ZSM-5, and H-[Al]ZSM-5. On each of the molecular sieves, the differential heats of adsorption for both ammonia and pyridine were constant up to a coverage of one per Bronsted site. Within experimental uncertainty, the differential heats at coverages below 1:1 were identical on each of the materials, with values for ammonia of 145 +/- 5 kJ/mol on H-[Fe]ZSM-5, 150 +/- 5 kJ/mol on H-[Ga]ZSM-5, and 145 +/- 5 kJ/mol on H-[Al]ZSM-5 and for pyridine of 195 +/- 5 kJ/mol on H-[Fe]ZSM-5, 200 +/- 5 kJ/mol on H-[Ga]ZSM-5, and 200 +/- 5 kJ/mol on H-[Al]ZSM-5. However, while specific rates for n-hexane cracking at 700 and 750 K and propene oligomerization at room temperature were nearly identical for H-[Ga]ZSM-5 and H-[Al]ZSM-5, the reactivity of the Bronsted sites in H-[Fe]ZSM-5 for each of the reactions is much lower. The implications of these results for the characterization of acidity in solid acids are discussed.
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页码:8745 / 8749
页数:5
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