Effects of Bronsted acidity in the mechanism of selective oxidation of propane to acetone on CaY zeolite at room temperature.

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

doi:10.1016/j.jcat.2005.04.004

Effects of Bronsted acidity in the mechanism of selective oxidation of propane to acetone on CaY zeolite at room temperature.

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

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

10 Citations (Scopus)

Abstract

The importance of Brønsted acid sites for partial oxidation of propane to acetone in CaY was investigated by in situ FTIR spectroscopy. With an increasing number of protons in Ca-Y, Volcano plots were observed for (1) amount of adsorbed propane; (2) initial acetone formation rate; (3) total amount of acetone after 20 h of reaction; (4) acetone selectivity. The results clearly show that Brønsted acidity increases the isopropylhydroperoxide (IHP) formation rate, most likely via a catalytic H+ transfer, and IHP decomposition into acetone and water. Moreover, with increasing IHP concentration 2-propanol was found in addition to acetone. Since an increasing number of Brønsted acid sites implies a decreasing number of Ca2+ in the zeolite, an optimal H+/Ca2+ ratio was observed for both activity and selectivity for acetone

Original language	Undefined
Pages (from-to)	411-423
Number of pages	13
Journal	Journal of catalysis
Volume	232
Issue number	2
DOIs	https://doi.org/10.1016/j.jcat.2005.04.004
Publication status	Published - 2005

Keywords

IR-54138
METIS-227828

Access to Document

10.1016/j.jcat.2005.04.004

Cite this

@article{7d42d6f2be23460bb59fe8de96acc34b,

title = "Effects of Bronsted acidity in the mechanism of selective oxidation of propane to acetone on CaY zeolite at room temperature.",

abstract = "The importance of Br{\o}nsted acid sites for partial oxidation of propane to acetone in CaY was investigated by in situ FTIR spectroscopy. With an increasing number of protons in Ca-Y, Volcano plots were observed for (1) amount of adsorbed propane; (2) initial acetone formation rate; (3) total amount of acetone after 20 h of reaction; (4) acetone selectivity. The results clearly show that Br{\o}nsted acidity increases the isopropylhydroperoxide (IHP) formation rate, most likely via a catalytic H+ transfer, and IHP decomposition into acetone and water. Moreover, with increasing IHP concentration 2-propanol was found in addition to acetone. Since an increasing number of Br{\o}nsted acid sites implies a decreasing number of Ca2+ in the zeolite, an optimal H+/Ca2+ ratio was observed for both activity and selectivity for acetone",

keywords = "IR-54138, METIS-227828",

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

year = "2005",

doi = "10.1016/j.jcat.2005.04.004",

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pages = "411--423",

journal = "Journal of catalysis",

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TY - JOUR

T1 - Effects of Bronsted acidity in the mechanism of selective oxidation of propane to acetone on CaY zeolite at room temperature.

AU - Xu, J.

AU - Mojet, Barbara

AU - van Ommen, J.G.

AU - Lefferts, Leonardus

PY - 2005

Y1 - 2005

N2 - The importance of Brønsted acid sites for partial oxidation of propane to acetone in CaY was investigated by in situ FTIR spectroscopy. With an increasing number of protons in Ca-Y, Volcano plots were observed for (1) amount of adsorbed propane; (2) initial acetone formation rate; (3) total amount of acetone after 20 h of reaction; (4) acetone selectivity. The results clearly show that Brønsted acidity increases the isopropylhydroperoxide (IHP) formation rate, most likely via a catalytic H+ transfer, and IHP decomposition into acetone and water. Moreover, with increasing IHP concentration 2-propanol was found in addition to acetone. Since an increasing number of Brønsted acid sites implies a decreasing number of Ca2+ in the zeolite, an optimal H+/Ca2+ ratio was observed for both activity and selectivity for acetone

AB - The importance of Brønsted acid sites for partial oxidation of propane to acetone in CaY was investigated by in situ FTIR spectroscopy. With an increasing number of protons in Ca-Y, Volcano plots were observed for (1) amount of adsorbed propane; (2) initial acetone formation rate; (3) total amount of acetone after 20 h of reaction; (4) acetone selectivity. The results clearly show that Brønsted acidity increases the isopropylhydroperoxide (IHP) formation rate, most likely via a catalytic H+ transfer, and IHP decomposition into acetone and water. Moreover, with increasing IHP concentration 2-propanol was found in addition to acetone. Since an increasing number of Brønsted acid sites implies a decreasing number of Ca2+ in the zeolite, an optimal H+/Ca2+ ratio was observed for both activity and selectivity for acetone

KW - IR-54138

KW - METIS-227828

U2 - 10.1016/j.jcat.2005.04.004

DO - 10.1016/j.jcat.2005.04.004

M3 - Article

VL - 232

SP - 411

EP - 423

JO - Journal of catalysis

JF - Journal of catalysis

SN - 0021-9517

IS - 2

ER -