A comparative study of the catalytic oxidation of chlorobenzene and toluene over Ce-Mn oxides

Yu Wang, Wei Deng, Yifu Wang, Limin Guo, Tatsumi Ishihara

Research output: Contribution to journalArticle

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Abstract

The morphology effects on the activity and stability of Ce-Mn oxide catalysts for chlorobenzene (CB) and toluene oxidation were compared and investigated in this work. Ce-Mn nano-sheets (CM–S), nano-particles (CM–P) and nano-rods (CM–R) were firstly prepared. The obvious morphology effects on the reactions were observed: the activity for toluene oxidation followed the order of CM–S > CM–P > CM–R. In contrast, the activity for CB oxidation followed the order of CM–R > CM–P > CM–S. For toluene oxidation, toluene adsorption and the C–H bond dissociation occurred at lower temperatures on the CM–S catalyst. The experimental results demonstrated that the higher content of surface adsorbed oxygen species and oxygen vacancies, as well as the enhanced Olatt species mobility of the CM–S catalyst were responsible for its highest catalytic activity. For CB oxidation, inactive planar CB adsorption on the 2D surface of CM–S catalyst and the strongly adsorbed Cl species from the CB decomposition resulted in serious deactivation of the catalyst. On the other hand, CB adsorption and the C-Cl bond dissociation occurred at lower temperatures on the CM–R catalyst, Cl-contained species can be easily removed during the Deacon Reaction and gas phase oxygen can be adsorbed on the CM–R surface to replenish the consumed oxygen, resulting in the improved activity and stability. These results showed that the catalytic performance of Ce-Mn oxides for CB and toluene oxidation was greatly affected by their morphologies.

Original languageEnglish
Pages (from-to)61-70
Number of pages10
JournalMolecular Catalysis
Volume459
DOIs
Publication statusPublished - Nov 1 2018

Fingerprint

chlorobenzenes
Catalytic oxidation
Toluene
Oxides
toluene
Cytidine Monophosphate
Oxidation
oxidation
Catalysts
oxides
rods
catalysts
Adsorption
oxygen
Oxygen
adsorption
dissociation
Oxygen vacancies
chlorobenzene
Catalyst activity

All Science Journal Classification (ASJC) codes

  • Catalysis
  • Process Chemistry and Technology
  • Physical and Theoretical Chemistry

Cite this

A comparative study of the catalytic oxidation of chlorobenzene and toluene over Ce-Mn oxides. / Wang, Yu; Deng, Wei; Wang, Yifu; Guo, Limin; Ishihara, Tatsumi.

In: Molecular Catalysis, Vol. 459, 01.11.2018, p. 61-70.

Research output: Contribution to journalArticle

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AB - The morphology effects on the activity and stability of Ce-Mn oxide catalysts for chlorobenzene (CB) and toluene oxidation were compared and investigated in this work. Ce-Mn nano-sheets (CM–S), nano-particles (CM–P) and nano-rods (CM–R) were firstly prepared. The obvious morphology effects on the reactions were observed: the activity for toluene oxidation followed the order of CM–S > CM–P > CM–R. In contrast, the activity for CB oxidation followed the order of CM–R > CM–P > CM–S. For toluene oxidation, toluene adsorption and the C–H bond dissociation occurred at lower temperatures on the CM–S catalyst. The experimental results demonstrated that the higher content of surface adsorbed oxygen species and oxygen vacancies, as well as the enhanced Olatt species mobility of the CM–S catalyst were responsible for its highest catalytic activity. For CB oxidation, inactive planar CB adsorption on the 2D surface of CM–S catalyst and the strongly adsorbed Cl species from the CB decomposition resulted in serious deactivation of the catalyst. On the other hand, CB adsorption and the C-Cl bond dissociation occurred at lower temperatures on the CM–R catalyst, Cl-contained species can be easily removed during the Deacon Reaction and gas phase oxygen can be adsorbed on the CM–R surface to replenish the consumed oxygen, resulting in the improved activity and stability. These results showed that the catalytic performance of Ce-Mn oxides for CB and toluene oxidation was greatly affected by their morphologies.

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