Desilication of highly siliceous zeolite ZSM-5 with NaOH and NaOH/tetrabutylamine hydroxide

2013
journal article
article
126
cris.lastimport.wos2024-04-09T22:55:17Z
dc.abstract.enThe results of both chemical and XPS analysis pointed out that desilication of highly siliceous ZSM-5 of Si/Al = 164 was more effective in the surface zone than in the bulk, contrary to zeolite ZSM-5 of Si/Al = 31.6. According to the IR studies in parent zeolite the concentration of protonic sites was very close to the concentration of Al indicating that all Al atoms can form Si-OH-Al. The results of our quantitative IR studies strongly support the realumination thesis, i.e. some Al atoms extracted in basic solutions are subsequently reinserted forming new acidic hydroxyls. In desilicated zeolites all Al atoms were able to form protonic sites, however part of them dehydroxylated during the activation of zeolite producing Lewis acid sites according to the stoichiometry: one protonic site was transformed into one Lewis site. Low temperature nitrogen adsorption revealed that the alkaline treatment of highly siliceous zeolite with 0.2 M NaOH/TBAOH mixture produced mesopores of smaller diameter and narrower pore size distribution than in the case of zeolite of medium Si/Al ratio. This result can be explained by low concentration of Al which similarly as TBA+ cations plays the role of pore directing agents (PDA). Contrary to TBA+, the presence of Al in desilication mixture, led to the formation of larger pores. Therefore, in highly siliceous zeolite TBA + played dominant role as PDA producing narrower pores. Highly siliceous zeolite with uniform distribution of relatively narrow pores may be useful catalyst or catalyst support. The influence of desilication temperature on porosity development was also investigated. The increase of desilication temperature from 338 to 353 K resulted in both more extensive demetalation (more Si and Al is extracted) and the distinct increase of the volume and surface of mesopores. Both lower concentration of protonic sites and higher concentration of Lewis sites confirmed partial zeolite destruction upon desilication at elevated temperature. The experiments of pivalonitrile sorption followed by IR spectroscopy showed a significant increase of accessibility of acid sites to bulky pivalonitrile molecules.pl
dc.affiliationWydział Chemii : Zakład Chemii Nieorganicznejpl
dc.affiliationWydział Chemii : Zakład Technologii Chemicznejpl
dc.affiliationWydział Chemii : Pracownia Spektrometrii w Podczerwienipl
dc.contributor.authorTarach, Karolina - 103685 pl
dc.contributor.authorGóra-Marek, Kinga - 128133 pl
dc.contributor.authorDrozdek, Marek - 127763 pl
dc.contributor.authorKuśtrowski, Piotr - 129800 pl
dc.contributor.authorDatka, Jerzy - 127692 pl
dc.contributor.authorMartínez Triguero, Joaquínpl
dc.contributor.authorRey, Fernandopl
dc.date.accessioned2015-01-23T08:39:24Z
dc.date.available2015-01-23T08:39:24Z
dc.date.issued2013pl
dc.description.additionalNa publikacji autorka Tarach Karolina podpisana jako Sadowska Karolina.pl
dc.description.admin[AB] Datka, Jerzy [SAP11003748] 50000141pl
dc.description.physical195-205pl
dc.description.volume168pl
dc.identifier.doi10.1016/j.micromeso.2012.09.033pl
dc.identifier.eissn1873-3093pl
dc.identifier.issn1387-1811pl
dc.identifier.urihttp://ruj.uj.edu.pl/xmlui/handle/item/2686
dc.languageengpl
dc.language.containerengpl
dc.rightsDodaję tylko opis bibliograficzny*
dc.rights.licencebez licencji
dc.rights.uri*
dc.subject.endesilicationpl
dc.subject.enrealuminationpl
dc.subject.enhighly siliceous zeolitepl
dc.subject.enIR spectroscopypl
dc.subject.enaccessibilitypl
dc.subject.encrackingpl
dc.subtypeArticlepl
dc.titleDesilication of highly siliceous zeolite ZSM-5 with NaOH and NaOH/tetrabutylamine hydroxidepl
dc.title.journalMicroporous and Mesoporous Materialspl
dc.typeJournalArticlepl
dspace.entity.typePublication
cris.lastimport.wos
2024-04-09T22:55:17Z
dc.abstract.enpl
The results of both chemical and XPS analysis pointed out that desilication of highly siliceous ZSM-5 of Si/Al = 164 was more effective in the surface zone than in the bulk, contrary to zeolite ZSM-5 of Si/Al = 31.6. According to the IR studies in parent zeolite the concentration of protonic sites was very close to the concentration of Al indicating that all Al atoms can form Si-OH-Al. The results of our quantitative IR studies strongly support the realumination thesis, i.e. some Al atoms extracted in basic solutions are subsequently reinserted forming new acidic hydroxyls. In desilicated zeolites all Al atoms were able to form protonic sites, however part of them dehydroxylated during the activation of zeolite producing Lewis acid sites according to the stoichiometry: one protonic site was transformed into one Lewis site. Low temperature nitrogen adsorption revealed that the alkaline treatment of highly siliceous zeolite with 0.2 M NaOH/TBAOH mixture produced mesopores of smaller diameter and narrower pore size distribution than in the case of zeolite of medium Si/Al ratio. This result can be explained by low concentration of Al which similarly as TBA+ cations plays the role of pore directing agents (PDA). Contrary to TBA+, the presence of Al in desilication mixture, led to the formation of larger pores. Therefore, in highly siliceous zeolite TBA + played dominant role as PDA producing narrower pores. Highly siliceous zeolite with uniform distribution of relatively narrow pores may be useful catalyst or catalyst support. The influence of desilication temperature on porosity development was also investigated. The increase of desilication temperature from 338 to 353 K resulted in both more extensive demetalation (more Si and Al is extracted) and the distinct increase of the volume and surface of mesopores. Both lower concentration of protonic sites and higher concentration of Lewis sites confirmed partial zeolite destruction upon desilication at elevated temperature. The experiments of pivalonitrile sorption followed by IR spectroscopy showed a significant increase of accessibility of acid sites to bulky pivalonitrile molecules.
dc.affiliationpl
Wydział Chemii : Zakład Chemii Nieorganicznej
dc.affiliationpl
Wydział Chemii : Zakład Technologii Chemicznej
dc.affiliationpl
Wydział Chemii : Pracownia Spektrometrii w Podczerwieni
dc.contributor.authorpl
Tarach, Karolina - 103685
dc.contributor.authorpl
Góra-Marek, Kinga - 128133
dc.contributor.authorpl
Drozdek, Marek - 127763
dc.contributor.authorpl
Kuśtrowski, Piotr - 129800
dc.contributor.authorpl
Datka, Jerzy - 127692
dc.contributor.authorpl
Martínez Triguero, Joaquín
dc.contributor.authorpl
Rey, Fernando
dc.date.accessioned
2015-01-23T08:39:24Z
dc.date.available
2015-01-23T08:39:24Z
dc.date.issuedpl
2013
dc.description.additionalpl
Na publikacji autorka Tarach Karolina podpisana jako Sadowska Karolina.
dc.description.adminpl
[AB] Datka, Jerzy [SAP11003748] 50000141
dc.description.physicalpl
195-205
dc.description.volumepl
168
dc.identifier.doipl
10.1016/j.micromeso.2012.09.033
dc.identifier.eissnpl
1873-3093
dc.identifier.issnpl
1387-1811
dc.identifier.uri
http://ruj.uj.edu.pl/xmlui/handle/item/2686
dc.languagepl
eng
dc.language.containerpl
eng
dc.rights*
Dodaję tylko opis bibliograficzny
dc.rights.licence
bez licencji
dc.rights.uri*
dc.subject.enpl
desilication
dc.subject.enpl
realumination
dc.subject.enpl
highly siliceous zeolite
dc.subject.enpl
IR spectroscopy
dc.subject.enpl
accessibility
dc.subject.enpl
cracking
dc.subtypepl
Article
dc.titlepl
Desilication of highly siliceous zeolite ZSM-5 with NaOH and NaOH/tetrabutylamine hydroxide
dc.title.journalpl
Microporous and Mesoporous Materials
dc.typepl
JournalArticle
dspace.entity.type
Publication

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