Comparison of catalytic properties of supported metal oxides for benzene oxidation using ozone

Hisahiro Einaga, Nanako Maeda, Yusuke Nagai

Research output: Contribution to journalArticle

14 Citations (Scopus)

Abstract

Catalytic oxidation of gaseous benzene using ozone over SiO2-supported metal oxides (oxides of Mn, Fe, Co, Ni, and Cu) was performed at 343 K. The supported metal oxides were prepared from metal nitrates via impregnation followed by calcination at 873 K. X-ray diffraction studies revealed that aggregated metal oxides were formed on the supports. The quantities of the exposed metal oxides on SiO2 were determined using temperature-programmed desorption of formic acid species adsorbed on the catalysts. The turnover frequencies (TOFs) for ozone decomposition and catalytic oxidation of benzene with ozone were also compared for the supported metal oxides. The TOFs for ozone decomposition with the supported metal oxides decreased in the order: Cu > Co ~ Ni > Fe > Mn. Conversely, the SiO2-supported Mn oxide (Mn/SiO2) catalyst exhibited the highest activity for catalytic oxidation of benzene with ozone and the highest efficiency for ozone utilization. FTIR studies revealed that benzene ring cleavage continuously proceeded on the Mn/SiO2 catalyst, and oxygen-containing species, which were readily oxidized to CO2 and CO in the presence of ozone, accumulated on the catalyst surface. The Fe-, Co-, Ni-, and Cu-oxides suffered from catalyst deactivation due to the build-up of by-product compounds, which was attributed to their low activity for oxidation of these substances. These results suggest that the most important steps in benzene oxidation with ozone on metal oxides are the formation and oxidation of by-product compounds. The higher activity of the Mn oxide catalyst for benzene oxidation is ascribed to the facile oxidation of these by-product compounds.

Original languageEnglish
Pages (from-to)3147-3158
Number of pages12
JournalCatalysis Science and Technology
Volume5
Issue number6
DOIs
Publication statusPublished - Jun 1 2015

Fingerprint

Ozone
Oxides
Benzene
Metals
Oxidation
Catalytic oxidation
Catalysts
Byproducts
formic acid
benzene oxide
Decomposition
Catalyst deactivation
Formic acid
Carbon Monoxide
Temperature programmed desorption
Impregnation
Nitrates
Calcination
Thermodynamic properties
Oxygen

All Science Journal Classification (ASJC) codes

  • Catalysis

Cite this

Comparison of catalytic properties of supported metal oxides for benzene oxidation using ozone. / Einaga, Hisahiro; Maeda, Nanako; Nagai, Yusuke.

In: Catalysis Science and Technology, Vol. 5, No. 6, 01.06.2015, p. 3147-3158.

Research output: Contribution to journalArticle

@article{394fb9e9a1704cfeb515c7a68d2dd6f6,
title = "Comparison of catalytic properties of supported metal oxides for benzene oxidation using ozone",
abstract = "Catalytic oxidation of gaseous benzene using ozone over SiO2-supported metal oxides (oxides of Mn, Fe, Co, Ni, and Cu) was performed at 343 K. The supported metal oxides were prepared from metal nitrates via impregnation followed by calcination at 873 K. X-ray diffraction studies revealed that aggregated metal oxides were formed on the supports. The quantities of the exposed metal oxides on SiO2 were determined using temperature-programmed desorption of formic acid species adsorbed on the catalysts. The turnover frequencies (TOFs) for ozone decomposition and catalytic oxidation of benzene with ozone were also compared for the supported metal oxides. The TOFs for ozone decomposition with the supported metal oxides decreased in the order: Cu > Co ~ Ni > Fe > Mn. Conversely, the SiO2-supported Mn oxide (Mn/SiO2) catalyst exhibited the highest activity for catalytic oxidation of benzene with ozone and the highest efficiency for ozone utilization. FTIR studies revealed that benzene ring cleavage continuously proceeded on the Mn/SiO2 catalyst, and oxygen-containing species, which were readily oxidized to CO2 and CO in the presence of ozone, accumulated on the catalyst surface. The Fe-, Co-, Ni-, and Cu-oxides suffered from catalyst deactivation due to the build-up of by-product compounds, which was attributed to their low activity for oxidation of these substances. These results suggest that the most important steps in benzene oxidation with ozone on metal oxides are the formation and oxidation of by-product compounds. The higher activity of the Mn oxide catalyst for benzene oxidation is ascribed to the facile oxidation of these by-product compounds.",
author = "Hisahiro Einaga and Nanako Maeda and Yusuke Nagai",
year = "2015",
month = "6",
day = "1",
doi = "10.1039/c5cy00315f",
language = "English",
volume = "5",
pages = "3147--3158",
journal = "Catalysis Science and Technology",
issn = "2044-4753",
publisher = "Royal Society of Chemistry",
number = "6",

}

TY - JOUR

T1 - Comparison of catalytic properties of supported metal oxides for benzene oxidation using ozone

AU - Einaga, Hisahiro

AU - Maeda, Nanako

AU - Nagai, Yusuke

PY - 2015/6/1

Y1 - 2015/6/1

N2 - Catalytic oxidation of gaseous benzene using ozone over SiO2-supported metal oxides (oxides of Mn, Fe, Co, Ni, and Cu) was performed at 343 K. The supported metal oxides were prepared from metal nitrates via impregnation followed by calcination at 873 K. X-ray diffraction studies revealed that aggregated metal oxides were formed on the supports. The quantities of the exposed metal oxides on SiO2 were determined using temperature-programmed desorption of formic acid species adsorbed on the catalysts. The turnover frequencies (TOFs) for ozone decomposition and catalytic oxidation of benzene with ozone were also compared for the supported metal oxides. The TOFs for ozone decomposition with the supported metal oxides decreased in the order: Cu > Co ~ Ni > Fe > Mn. Conversely, the SiO2-supported Mn oxide (Mn/SiO2) catalyst exhibited the highest activity for catalytic oxidation of benzene with ozone and the highest efficiency for ozone utilization. FTIR studies revealed that benzene ring cleavage continuously proceeded on the Mn/SiO2 catalyst, and oxygen-containing species, which were readily oxidized to CO2 and CO in the presence of ozone, accumulated on the catalyst surface. The Fe-, Co-, Ni-, and Cu-oxides suffered from catalyst deactivation due to the build-up of by-product compounds, which was attributed to their low activity for oxidation of these substances. These results suggest that the most important steps in benzene oxidation with ozone on metal oxides are the formation and oxidation of by-product compounds. The higher activity of the Mn oxide catalyst for benzene oxidation is ascribed to the facile oxidation of these by-product compounds.

AB - Catalytic oxidation of gaseous benzene using ozone over SiO2-supported metal oxides (oxides of Mn, Fe, Co, Ni, and Cu) was performed at 343 K. The supported metal oxides were prepared from metal nitrates via impregnation followed by calcination at 873 K. X-ray diffraction studies revealed that aggregated metal oxides were formed on the supports. The quantities of the exposed metal oxides on SiO2 were determined using temperature-programmed desorption of formic acid species adsorbed on the catalysts. The turnover frequencies (TOFs) for ozone decomposition and catalytic oxidation of benzene with ozone were also compared for the supported metal oxides. The TOFs for ozone decomposition with the supported metal oxides decreased in the order: Cu > Co ~ Ni > Fe > Mn. Conversely, the SiO2-supported Mn oxide (Mn/SiO2) catalyst exhibited the highest activity for catalytic oxidation of benzene with ozone and the highest efficiency for ozone utilization. FTIR studies revealed that benzene ring cleavage continuously proceeded on the Mn/SiO2 catalyst, and oxygen-containing species, which were readily oxidized to CO2 and CO in the presence of ozone, accumulated on the catalyst surface. The Fe-, Co-, Ni-, and Cu-oxides suffered from catalyst deactivation due to the build-up of by-product compounds, which was attributed to their low activity for oxidation of these substances. These results suggest that the most important steps in benzene oxidation with ozone on metal oxides are the formation and oxidation of by-product compounds. The higher activity of the Mn oxide catalyst for benzene oxidation is ascribed to the facile oxidation of these by-product compounds.

UR - http://www.scopus.com/inward/record.url?scp=84930630113&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=84930630113&partnerID=8YFLogxK

U2 - 10.1039/c5cy00315f

DO - 10.1039/c5cy00315f

M3 - Article

AN - SCOPUS:84930630113

VL - 5

SP - 3147

EP - 3158

JO - Catalysis Science and Technology

JF - Catalysis Science and Technology

SN - 2044-4753

IS - 6

ER -