On the role of strength and location of Bronsted acid sites for ethylaminesynthesis on mordenite catalysts

Citation
Va. Veefkind et al., On the role of strength and location of Bronsted acid sites for ethylaminesynthesis on mordenite catalysts, APP CATAL A, 194, 2000, pp. 319-332
Citations number
39
Categorie Soggetti
Physical Chemistry/Chemical Physics","Chemical Engineering
Journal title
APPLIED CATALYSIS A-GENERAL
ISSN journal
0926860X → ACNP
Volume
194
Year of publication
2000
Pages
319 - 332
Database
ISI
SICI code
0926-860X(20000313)194:<319:OTROSA>2.0.ZU;2-W
Abstract
The elementary steps of alkylation of ammonia with ethanol and the role:of the strength and location of the acid sites of the mordenite catalysts were investigated by means of in situ i.r. spectroscopy, temperature-programmed desorption and kinetic measurements. Ethanol and ammonia have access to al l Bronsted acid sites of the mordenites investigated. From the products onl y monoethylamine reached all acid sites, while di- and triethylamine sorbed only on 60% and 45% of the sites, respectively. The Bronsted acid sites of HNa-mordenites are exclusively located in the main channel up to an hydrog en exchange degree of 60%. Only at higher exchange degrees are the sites in the side pockets also exchanged. These latter acid sites apparently contri bute significantly to the overall rate of amination. Mordenite with a high concentration of Na+ ions (low H+ exchange degree) stabilize ammonium less than those with a low Na+ concentration. This leads to more ethene produced dukng: the amination reaction. While some diethyl ether is:formed during a mination, the alcohol and not the ether is the primary alkylating agent. (C ) 2000 Elsevier Science B,V. All rights reserved.