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    Catalytic performance of Pd catalyst supported on Zr:Ce modified mesoporous silica for methane oxidation

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    790.8Kb
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    Description:
    Accepted manuscript
    Embargo End Date:
    2022-05-19
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    Type
    Article
    Authors
    Khan, Hassnain Abbas cc
    Hao, Junyu
    Farooq, Aamir cc
    KAUST Department
    Chemical Kinetics & Laser Sensors Laboratory
    Clean Combustion Research Center
    Mechanical Engineering
    Mechanical Engineering Program
    Physical Science and Engineering (PSE) Division
    Date
    2020-05-15
    Online Publication Date
    2020-05-15
    Print Publication Date
    2020-10
    Embargo End Date
    2022-05-19
    Submitted Date
    2020-03-26
    Permanent link to this record
    http://hdl.handle.net/10754/662942
    
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    Abstract
    Catalytic oxidation of methane is critical for exhaust after-treatment systems where cold-start emissions and lean combustion still pose serious challenges. In this work, the effect of support materials on the complete catalytic oxidation of methane over palladium is studied in dry and wet conditions. A series of metal oxides (CeO2, ZrO2, n-SiO2) and mixed metal oxides (Zr0.65Ce0.35O2, Zr0.33Ce0.33/n-Si0.33O2, Zr0.66Ce0.17/n-Si0.17O2) supported Pd catalysts were synthesized, characterized and tested for methane oxidation. Pd/n-SiO2 was found to be highly active catalyst with the lowest initial (T10%) and final (T100%) conversion temperatures as compared to Pd supported on CeO2 and ZrO2. Methane combustion over mixed oxide supports, prepared with different ratios of Zr:Ce:Si, showed improved catalytic performance. Catalyst with equal ratios of Zr:Ce:Si (Pd/Zr0.33Ce0.33/n-Si0.33O2) showed similar performance to that of Pd/n-SiO2 with approximately ~8 (±2) °C higher light-off temperature. Additionally, cyclic wet (8 vol% H2O) and dry reactions were performed to evaluate the hydrothermal stability and activity regeneration when switching from wet to dry conditions. Optimal addition of ZrO2 and CeO2 to n-SiO2 resulted in higher stability of palladium catalyst over wide ranges of temperatures (350–600 °C). Catalysts were characterized by various analytical techniques, including TEM, XRD, XRF, N2-BET, O2-TPD, and CO chemisorption. TEM results demonstrate that mixed oxide support stabilized Pd nanoparticles, and n-SiO2 encapsulation prevented sintering and deactivation. Activity tests and characterization results demonstrate overall superior catalytic properties of Pd supported on Zr0.33Ce0.33/n-Si0.33O2. This catalyst can be quite promising for practical applications due to its high activity for total methane oxidation and excellent thermal stability.
    Citation
    Khan, H. A., Hao, J., & Farooq, A. (2020). Catalytic performance of Pd catalyst supported on Zr:Ce modified mesoporous silica for methane oxidation. Chemical Engineering Journal, 397, 125489. doi:10.1016/j.cej.2020.125489
    Sponsors
    Research reported in this work was funded by the Office of Sponsored Research at King Abdullah University of Science and Technology (KAUST) under the Competitive Research Grant # CRG-3402.
    Publisher
    Elsevier BV
    Journal
    Chemical Engineering Journal
    DOI
    10.1016/j.cej.2020.125489
    Additional Links
    https://linkinghub.elsevier.com/retrieve/pii/S138589472031617X
    ae974a485f413a2113503eed53cd6c53
    10.1016/j.cej.2020.125489
    Scopus Count
    Collections
    Articles; Physical Science and Engineering (PSE) Division; Mechanical Engineering Program; Clean Combustion Research Center

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