Observation of a compensation relation for n-hexane adsorption in zeolites with different structures:: implications for catalytic activity

被引:56
|
作者
Ramachandran, CE
Williams, BA
van Bokhoven, JA
Miller, JT
机构
[1] BP Res Ctr, Naperville, IL 60563 USA
[2] Innovene, Naperville, IL 60563 USA
[3] ETH, Swiss Fed Inst Technol, Inst Chem & Bioengn, CH-8093 Zurich, Switzerland
关键词
compensation effect; enthalpy of n-hexane adsorption in zeolites; Henry's constant for n-hexane on zeolites; zeolite acidity; alkane sorption; MFI; Y zeolite; mordenite; beta zeofite; intrinsic zeolite activity;
D O I
10.1016/j.jcat.2005.04.017
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
The Henry's equilibrium constant and enthalpy of n-hexane adsorption at low coverage have been determined at 423 K for zeolites of different structural types that have been subjected to different treatments, The Henry's constant and enthalpy of adsorption increased as the pore size decreased as MFI > MOR > BEA > FAU. Bronsted acid sites and non-framework At produced through steaming gave smaller increases, and changes due to alkali or lanthanide ions had little effect. From the enthalpy of adsorption and (lie Henry's equilibrium constant, the entropy of adsorption was calculated. Despite the large differences in structure and composition of the zeolites. there is a linear correlation, or compensation relation, between the entropy and enthalpy of adsorption for all of the zeolites. Combined with previous work in which the same zeolites exhibited a linear kinetic compensation. or Constable relation, for the monomolecular cracking of n-hexane, these results support the proposal that the intrinsic acid strengths of active Bronsted acid sites in zeolites of different structures or silica-to-alumina ratios with Lewis acid sites from nonframework Al are similar. (c) 2005 Published by Elsevier Inc.
引用
收藏
页码:100 / 108
页数:9
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