Relationship between acidity and catalytic reactivity of Faujasite Zeolite: a periodic DFT study

C. Liu, G. Li, E.J.M. Hensen, E.A. Pidko

Research output: Contribution to journalArticleAcademicpeer-review

22 Citations (Scopus)
6 Downloads (Pure)

Abstract

The fundamental aspects of Brønsted acidity and catalytic reactivity of faujasite-type zeolites were investigated by periodic DFT calculations. The adsorption energies of ammonia and pyridine on the Brønsted acid site (BAS) were used to determine the acidity. It is demonstrated that the acid strength of zeolite materials increases with rising Si/Al ratio (low-silica faujasite), and then levels off at high Si/Al ratio (high-silica faujasite). The presence of multinuclear extra framework Al (EFAl) in the sodalite cages substantially enhances the Brønsted acidity. The catalytic reactivity of faujasite toward protolytic propane cracking correlates well with the characterized acidity by base adsorption. However, for H/D exchange reaction of benzene the presence of EFAl species can induce deviations between the measured acidity and the reactivity of faujasite catalysts, indicating that acidity and reactivity are not always directly correlated.
Original languageEnglish
Pages (from-to)570–577
JournalJournal of Catalysis
Volume344
DOIs
Publication statusPublished - 2016

Fingerprint

Zeolites
Acidity
Discrete Fourier transforms
acidity
reactivity
Silicon Dioxide
Silica
silicon dioxide
Adsorption
sodalite
Propane
acids
adsorption
Acids
Benzene
Ammonia
propane
zeolites
Pyridine
Strength of materials

Cite this

@article{01086bcc1e8b4689b78a278e2528ecc0,
title = "Relationship between acidity and catalytic reactivity of Faujasite Zeolite: a periodic DFT study",
abstract = "The fundamental aspects of Br{\o}nsted acidity and catalytic reactivity of faujasite-type zeolites were investigated by periodic DFT calculations. The adsorption energies of ammonia and pyridine on the Br{\o}nsted acid site (BAS) were used to determine the acidity. It is demonstrated that the acid strength of zeolite materials increases with rising Si/Al ratio (low-silica faujasite), and then levels off at high Si/Al ratio (high-silica faujasite). The presence of multinuclear extra framework Al (EFAl) in the sodalite cages substantially enhances the Br{\o}nsted acidity. The catalytic reactivity of faujasite toward protolytic propane cracking correlates well with the characterized acidity by base adsorption. However, for H/D exchange reaction of benzene the presence of EFAl species can induce deviations between the measured acidity and the reactivity of faujasite catalysts, indicating that acidity and reactivity are not always directly correlated.",
author = "C. Liu and G. Li and E.J.M. Hensen and E.A. Pidko",
year = "2016",
doi = "10.1016/j.jcat.2016.10.027",
language = "English",
volume = "344",
pages = "570–577",
journal = "Journal of Catalysis",
issn = "0021-9517",
publisher = "Academic Press Inc.",

}

Relationship between acidity and catalytic reactivity of Faujasite Zeolite : a periodic DFT study. / Liu, C.; Li, G.; Hensen, E.J.M.; Pidko, E.A.

In: Journal of Catalysis, Vol. 344, 2016, p. 570–577.

Research output: Contribution to journalArticleAcademicpeer-review

TY - JOUR

T1 - Relationship between acidity and catalytic reactivity of Faujasite Zeolite

T2 - a periodic DFT study

AU - Liu, C.

AU - Li, G.

AU - Hensen, E.J.M.

AU - Pidko, E.A.

PY - 2016

Y1 - 2016

N2 - The fundamental aspects of Brønsted acidity and catalytic reactivity of faujasite-type zeolites were investigated by periodic DFT calculations. The adsorption energies of ammonia and pyridine on the Brønsted acid site (BAS) were used to determine the acidity. It is demonstrated that the acid strength of zeolite materials increases with rising Si/Al ratio (low-silica faujasite), and then levels off at high Si/Al ratio (high-silica faujasite). The presence of multinuclear extra framework Al (EFAl) in the sodalite cages substantially enhances the Brønsted acidity. The catalytic reactivity of faujasite toward protolytic propane cracking correlates well with the characterized acidity by base adsorption. However, for H/D exchange reaction of benzene the presence of EFAl species can induce deviations between the measured acidity and the reactivity of faujasite catalysts, indicating that acidity and reactivity are not always directly correlated.

AB - The fundamental aspects of Brønsted acidity and catalytic reactivity of faujasite-type zeolites were investigated by periodic DFT calculations. The adsorption energies of ammonia and pyridine on the Brønsted acid site (BAS) were used to determine the acidity. It is demonstrated that the acid strength of zeolite materials increases with rising Si/Al ratio (low-silica faujasite), and then levels off at high Si/Al ratio (high-silica faujasite). The presence of multinuclear extra framework Al (EFAl) in the sodalite cages substantially enhances the Brønsted acidity. The catalytic reactivity of faujasite toward protolytic propane cracking correlates well with the characterized acidity by base adsorption. However, for H/D exchange reaction of benzene the presence of EFAl species can induce deviations between the measured acidity and the reactivity of faujasite catalysts, indicating that acidity and reactivity are not always directly correlated.

U2 - 10.1016/j.jcat.2016.10.027

DO - 10.1016/j.jcat.2016.10.027

M3 - Article

VL - 344

SP - 570

EP - 577

JO - Journal of Catalysis

JF - Journal of Catalysis

SN - 0021-9517

ER -