Propane selective oxidation on alkaline earth exchanged zeolite Y: room temperature in situ IR study

J. Xu; Barbara Mojet; J.G. van Ommen; Leonardus Lefferts

doi:10.1039/b305777c

Propane selective oxidation on alkaline earth exchanged zeolite Y: room temperature in situ IR study

J. Xu, Barbara Mojet, J.G. van Ommen, Leonardus Lefferts

Research output: Contribution to journal › Article › Academic › peer-review

22 Citations (Scopus)

Abstract

The effect of zeolite Y ion-exchanged with a series of alkaline-earth cations on selective propane oxidation at room temperature was studied with in situ infrared spectroscopy. Isopropylhydroperoxide was observed as a reaction intermediate and can be decomposed into acetone and water. Contrary to previous studies, BaY was found to be active at room temperature. The reaction rate increased in the order BaY<MgY<SrY<CaY based on the rate of formation of adsorbed acetone. Surprisingly, the acetone/water ratio was found to increase with cation size, while no other products could be detected. Moreover, the acetone/isopropylhydroperoxide ratio decreased with decreasing number of Brønsted acid sites. Both observations mark the importance of Brønsted acid sites for this reaction, in addition to alkali (earth) cations. A two-step mechanism with two different active sites is proposed. Conversion of propane into isopropylhydroperoxide takes place on cations, while the decomposition into acetone occurs by Brønsted acid sites.

Original language	Undefined
Pages (from-to)	4407-4413
Number of pages	7
Journal	Physical chemistry chemical physics
Volume	5
Issue number	20
DOIs	https://doi.org/10.1039/b305777c
Publication status	Published - 2003

Keywords

IR-40709
METIS-213898

Access to Document

10.1039/b305777c

Cite this

@article{24951d37e88140ffbdb3da065ba0576f,

title = "Propane selective oxidation on alkaline earth exchanged zeolite Y: room temperature in situ IR study",

abstract = "The effect of zeolite Y ion-exchanged with a series of alkaline-earth cations on selective propane oxidation at room temperature was studied with in situ infrared spectroscopy. Isopropylhydroperoxide was observed as a reaction intermediate and can be decomposed into acetone and water. Contrary to previous studies, BaY was found to be active at room temperature. The reaction rate increased in the order BaY<MgY<SrY<CaY based on the rate of formation of adsorbed acetone. Surprisingly, the acetone/water ratio was found to increase with cation size, while no other products could be detected. Moreover, the acetone/isopropylhydroperoxide ratio decreased with decreasing number of Br{\o}nsted acid sites. Both observations mark the importance of Br{\o}nsted acid sites for this reaction, in addition to alkali (earth) cations. A two-step mechanism with two different active sites is proposed. Conversion of propane into isopropylhydroperoxide takes place on cations, while the decomposition into acetone occurs by Br{\o}nsted acid sites.",

keywords = "IR-40709, METIS-213898",

author = "J. Xu and Barbara Mojet and {van Ommen}, J.G. and Leonardus Lefferts",

year = "2003",

doi = "10.1039/b305777c",

language = "Undefined",

volume = "5",

pages = "4407--4413",

journal = "Physical chemistry chemical physics",

issn = "1463-9076",

publisher = "Royal Society of Chemistry",

number = "20",

}

TY - JOUR

T1 - Propane selective oxidation on alkaline earth exchanged zeolite Y: room temperature in situ IR study

AU - Xu, J.

AU - Mojet, Barbara

AU - van Ommen, J.G.

AU - Lefferts, Leonardus

PY - 2003

Y1 - 2003

N2 - The effect of zeolite Y ion-exchanged with a series of alkaline-earth cations on selective propane oxidation at room temperature was studied with in situ infrared spectroscopy. Isopropylhydroperoxide was observed as a reaction intermediate and can be decomposed into acetone and water. Contrary to previous studies, BaY was found to be active at room temperature. The reaction rate increased in the order BaY<MgY<SrY<CaY based on the rate of formation of adsorbed acetone. Surprisingly, the acetone/water ratio was found to increase with cation size, while no other products could be detected. Moreover, the acetone/isopropylhydroperoxide ratio decreased with decreasing number of Brønsted acid sites. Both observations mark the importance of Brønsted acid sites for this reaction, in addition to alkali (earth) cations. A two-step mechanism with two different active sites is proposed. Conversion of propane into isopropylhydroperoxide takes place on cations, while the decomposition into acetone occurs by Brønsted acid sites.

AB - The effect of zeolite Y ion-exchanged with a series of alkaline-earth cations on selective propane oxidation at room temperature was studied with in situ infrared spectroscopy. Isopropylhydroperoxide was observed as a reaction intermediate and can be decomposed into acetone and water. Contrary to previous studies, BaY was found to be active at room temperature. The reaction rate increased in the order BaY<MgY<SrY<CaY based on the rate of formation of adsorbed acetone. Surprisingly, the acetone/water ratio was found to increase with cation size, while no other products could be detected. Moreover, the acetone/isopropylhydroperoxide ratio decreased with decreasing number of Brønsted acid sites. Both observations mark the importance of Brønsted acid sites for this reaction, in addition to alkali (earth) cations. A two-step mechanism with two different active sites is proposed. Conversion of propane into isopropylhydroperoxide takes place on cations, while the decomposition into acetone occurs by Brønsted acid sites.

KW - IR-40709

KW - METIS-213898

U2 - 10.1039/b305777c

DO - 10.1039/b305777c

M3 - Article

VL - 5

SP - 4407

EP - 4413

JO - Physical chemistry chemical physics

JF - Physical chemistry chemical physics

SN - 1463-9076

IS - 20

ER -