co3o4-ceo2氧化物对丙烷完全氧化的催化性能
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a State Key Laboratory of Fine Chemicals & Laboratory of Advanced Materials and Catalytic Engineering, Dalian University of Technology, Dalian 116024, Liaoning, China b Methanol to Olefins National Engineering Laboratory, Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China
ARTICLE INFO
Article history: Received 22 August 2019 Accepted 30 September 2019 Published 5 April 2020
Keywords: Propane Total oxidation Co3O4-CeO2 In-suit DRIFTS Volatile organic compounds
Arttic properties of Co3O4-CeO2 binary oxides for propane total oxidation
Wenjun Zhu a,b, Xiao Chen a, Jianhui Jin a, Xin Di a, Changhai Liang a,*, Zhongmin Liu b,#
Chinese Journal of Catalysis 41 (2020) 679–690
催化学报 2020年 第41卷 第4期 |
52
available at
journal homepage: /locate/chnjc
© 2020, Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. All rights reserved.
1. Introduction
Volatile organic compounds (VOCs), as the major contributors to global air pollution, have caused serious environmental problems in recent years. They are emitted from various sources, such as chemical plants, power stations, oil refineries, and vehicle exhausts [1]. Over time, environmental legislation on the permissible levels of atmospheric emission has become increasingly stringent; consequently, the usage of liquefied petroleum gas (LPG) and liquefied natural gas (LNG) as alternatives in gasoline and diesel vehicles is increasing. Moreover,
ABSTRACT
A series of Co3O4-CeO2 binary oxides with various Co/(Ce+Co) molar ratios were synthesized using a citric acid method, and their catalytic properties toward the total oxidation of propane were examined. The activities of the catalysts decrease in the order CoCeOx-70 > CoCeOx-90 > Co3O4 > CoCeOx-50 > CoCeOx-20 > CeO2. CoCeOx-70 (Co/(Ce+Co) = 70% molar ratio) exhibits the highest catalytic activity toward the total oxidation of propane, of which the T90 is 310 °C (GHSV = 120000 mL h1 g1), which is 25 °C lower than that of pure Co3O4. The enhancement of the catalytic performance of CoCeOx-70 is attributed to the strong interaction between CeO2 and Co3O4, the improvement of the low-temperature reducibility, and the increase in the number of active oxygen species. In-situ DRIFTS and reaction kinetics measurement reveal that Ce addition does not change the reaction mechanism, but promotes the adsorption and activation of propane on the catalyst surface. The addition of water vapor and CO2 in reactant gas has a negative effect on the propane conversion, and the catalyst is more sensitive to water vapor than to CO2. In addition, CoCeOx-70 exhibits excellent stability and reusability in water vapor and CO2 atmosphere.
ARTICLE INFO
Article history: Received 22 August 2019 Accepted 30 September 2019 Published 5 April 2020
Keywords: Propane Total oxidation Co3O4-CeO2 In-suit DRIFTS Volatile organic compounds
Arttic properties of Co3O4-CeO2 binary oxides for propane total oxidation
Wenjun Zhu a,b, Xiao Chen a, Jianhui Jin a, Xin Di a, Changhai Liang a,*, Zhongmin Liu b,#
Chinese Journal of Catalysis 41 (2020) 679–690
催化学报 2020年 第41卷 第4期 |
52
available at
journal homepage: /locate/chnjc
© 2020, Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. All rights reserved.
1. Introduction
Volatile organic compounds (VOCs), as the major contributors to global air pollution, have caused serious environmental problems in recent years. They are emitted from various sources, such as chemical plants, power stations, oil refineries, and vehicle exhausts [1]. Over time, environmental legislation on the permissible levels of atmospheric emission has become increasingly stringent; consequently, the usage of liquefied petroleum gas (LPG) and liquefied natural gas (LNG) as alternatives in gasoline and diesel vehicles is increasing. Moreover,
ABSTRACT
A series of Co3O4-CeO2 binary oxides with various Co/(Ce+Co) molar ratios were synthesized using a citric acid method, and their catalytic properties toward the total oxidation of propane were examined. The activities of the catalysts decrease in the order CoCeOx-70 > CoCeOx-90 > Co3O4 > CoCeOx-50 > CoCeOx-20 > CeO2. CoCeOx-70 (Co/(Ce+Co) = 70% molar ratio) exhibits the highest catalytic activity toward the total oxidation of propane, of which the T90 is 310 °C (GHSV = 120000 mL h1 g1), which is 25 °C lower than that of pure Co3O4. The enhancement of the catalytic performance of CoCeOx-70 is attributed to the strong interaction between CeO2 and Co3O4, the improvement of the low-temperature reducibility, and the increase in the number of active oxygen species. In-situ DRIFTS and reaction kinetics measurement reveal that Ce addition does not change the reaction mechanism, but promotes the adsorption and activation of propane on the catalyst surface. The addition of water vapor and CO2 in reactant gas has a negative effect on the propane conversion, and the catalyst is more sensitive to water vapor than to CO2. In addition, CoCeOx-70 exhibits excellent stability and reusability in water vapor and CO2 atmosphere.