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作者:

Chu, Peiqi (Chu, Peiqi.) | Wang, Saifei (Wang, Saifei.) | Zhang, Yi (Zhang, Yi.) | Zhao, Shiguang (Zhao, Shiguang.) | Wang, Yahan (Wang, Yahan.) | Deng, Jiguang (Deng, Jiguang.) | Duan, Erhong (Duan, Erhong.)

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摘要:

A novel La-Co-O-C (LC-C) composites were prepared via a facile co-hydrothermal route with oxides and glycerol and further optimized for methane catalytic activity and thermal stability via component regulation. It was demonstrated that Co3O4 phase was the main component in regulation. The combined results of X-ray photoelectron spectroscopy (XPS), temperature-programmed desorption of oxygen (O-2-TPD), temperature-programmed reduction of hydrogen (H-2-TPR), temperature-programmed desorption of ammonia/carbon dioxide (NH3/CO2-TPD) revealed that component regulation led to more oxygen vacancies and exposure of surface Co2+, lower surface basicity and optimized acidity, which were beneficial for adsorption of active oxygen species and activation of methane molecules, resulting in the excellent catalytic oxidation performance. Especially, the (3.5)LC-C (3.5 is Co-to-La molar ratio) showed the optimum activity and the T-50 and T-90 (the temperature at which the CH4 conversion rate was 50% and 90%, respectively) were 318 and 367 degrees C, respectively. Using theoretical calculations and in situ diffuse reflection infrared Fourier transform spectroscopy characterization, it was also found that the catalytic mechanism changes from the "Rideal-Eley" mechanism to the "Two-term" mechanism depending on the temperature windows in which the reaction takes place. Besides, the use of the "Flynn-Wall-Ozawa" model in thermoanalytical kinetics revealed that component regulation simultaneously optimized the decomposition activation energy, further expanding the application scope of carbon-containing composites. (C) 2022 The Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences. Published by Elsevier B.V.

关键词:

Component regulation Co3O4 Composite oxides Methane combustion

作者机构:

  • [ 1 ] [Chu, Peiqi]Hebei Univ Sci & Technol, Sch Environm Sci & Engn, Shijiazhuang 050018, Hebei, Peoples R China
  • [ 2 ] [Wang, Saifei]Hebei Univ Sci & Technol, Sch Environm Sci & Engn, Shijiazhuang 050018, Hebei, Peoples R China
  • [ 3 ] [Zhao, Shiguang]Hebei Univ Sci & Technol, Sch Environm Sci & Engn, Shijiazhuang 050018, Hebei, Peoples R China
  • [ 4 ] [Wang, Yahan]Hebei Univ Sci & Technol, Sch Environm Sci & Engn, Shijiazhuang 050018, Hebei, Peoples R China
  • [ 5 ] [Duan, Erhong]Hebei Univ Sci & Technol, Sch Environm Sci & Engn, Shijiazhuang 050018, Hebei, Peoples R China
  • [ 6 ] [Zhang, Yi]Hebei Univ Sci & Technol, Sch Chem & Pharmaceut Engn, Shijiazhuang 050018, Hebei, Peoples R China
  • [ 7 ] [Deng, Jiguang]Beijing Univ Technol, Coll Environm & Energy Engn, Beijing 100124, Peoples R China

通讯作者信息:

  • [Wang, Saifei]Hebei Univ Sci & Technol, Sch Environm Sci & Engn, Shijiazhuang 050018, Hebei, Peoples R China;;[Duan, Erhong]Hebei Univ Sci & Technol, Sch Environm Sci & Engn, Shijiazhuang 050018, Hebei, Peoples R China;;[Deng, Jiguang]Beijing Univ Technol, Coll Environm & Energy Engn, Beijing 100124, Peoples R China;;

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来源 :

JOURNAL OF ENVIRONMENTAL SCIENCES

ISSN: 1001-0742

年份: 2023

卷: 126

页码: 459-469

6 . 9 0 0

JCR@2022

ESI学科: ENVIRONMENT/ECOLOGY;

ESI高被引阀值:17

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