TY - JOUR
T1 - A comparative study of the catalytic oxidation of chlorobenzene and toluene over Ce-Mn oxides
AU - Wang, Yu
AU - Deng, Wei
AU - Wang, Yifu
AU - Guo, Limin
AU - Ishihara, Tatsumi
N1 - Funding Information:
The work was financiallysupported by the Huazhong University of Science and Technology, the Opening Project of State Key Laboratory of High Performance Ceramics and Superfine Microstructure (No. SKL201707SIC ) and China Postdoctoral Science Foundation (No. 2016M602303 ). The authors thank the Analysis and Testing Center of Huazhong University of Science and Technology for analytical support.
Publisher Copyright:
© 2018 Elsevier B.V.
PY - 2018/11
Y1 - 2018/11
N2 - 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.
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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U2 - 10.1016/j.mcat.2018.08.022
DO - 10.1016/j.mcat.2018.08.022
M3 - Article
AN - SCOPUS:85052882070
SN - 2468-8231
VL - 459
SP - 61
EP - 70
JO - Molecular Catalysis
JF - Molecular Catalysis
ER -