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    Optimizing Pd:Zn molar Ratio in PdZn/CeO2 for CO2 Hydrogenation to Methanol

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    Name:
    Ojelade et al.pdf
    Size:
    1.726Mb
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    PDF
    Description:
    Accepted manuscript
    Embargo End Date:
    2021-07-30
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    Type
    Article
    Authors
    Ojelade, Opeyemi A.
    Zaman, Sharif F. cc
    Daous, Muhammad A.
    Al-Zahrani, Abdulrahim A.
    Malik, Ali S. cc
    Driss, Hafedh
    Shterk, Genrikh cc
    Gascon, Jorge cc
    KAUST Department
    Advanced Catalytic Materials, KAUST Catalysis Center (KCC), King Abdullah University of Science and Technology, Thuwal, 23955, Saudi Arabia
    Chemical Engineering Program
    KAUST Catalysis Center (KCC)
    Physical Science and Engineering (PSE) Division
    KAUST Grant Number
    JP-19-001
    Date
    2019-07-30
    Online Publication Date
    2019-07-30
    Print Publication Date
    2019-07
    Embargo End Date
    2021-07-30
    Permanent link to this record
    http://hdl.handle.net/10754/656511
    
    Metadata
    Show full item record
    Abstract
    We report the compositional optimization of Pd:Zn/CeO2 catalysts prepared via sol-gel chelatization for the hydrogenation of CO2 under mild reaction conditions. The formation of a PdZn alloy, which is the main active phase for this reaction, was maximized for the catalyst with a Pd to Zn ratio close to 1. For this catalyst, a maximum conversion of 14%, close to thermodynamic equilibrium, and high selectivity to methanol (95%) were achieved at 220 °C, 20 bar, 2400 h−1 GHSV and H2:CO2 stoichiometric ratio of 3:1. The formation of PdZn alloys was achieved by reducing the catalyst precursor at 550 °C under hydrogen flow and confirmed by XRD. XPS study confirmed the presence of Pd°, being maximum for the optimized catalyst composition. At lower temperature, i.e. 180 °C, 1.0PdZn catalyst showed 100% selectivity to methanol with 8% CO2 conversion. RWGS reaction is responsible for the production of CO and its selectivity increases with temperature. In situ DRIFTS suggests that CO2 is activated as adsorbed CO3- species over CeO2. Surface micro-kinetics demonstrates that methanol can be formed either via formaldehyde or formic acid surface intermediates.
    Citation
    Ojelade, O. A., Zaman, S. F., Daous, M. A., Al-Zahrani, A. A., Malik, A. S., Driss, H., … Gascon, J. (2019). Optimizing Pd:Zn molar Ratio in PdZn/CeO2 for CO2 Hydrogenation to Methanol. Applied Catalysis A: General, 117185. doi:10.1016/j.apcata.2019.117185
    Sponsors
    This joint project was co-founded by King Abdulaziz University (KAU), Jeddah, and King Abdullah University of Science and Technology (KAUST), Thuwal, under grant number “JP-19-001”. The authors, therefore, acknowledge KAU and KAUST for their technical and financial support.
    Publisher
    Elsevier BV
    Journal
    Applied Catalysis A: General
    DOI
    10.1016/j.apcata.2019.117185
    Additional Links
    https://linkinghub.elsevier.com/retrieve/pii/S0926860X19303400
    ae974a485f413a2113503eed53cd6c53
    10.1016/j.apcata.2019.117185
    Scopus Count
    Collections
    Articles; Physical Science and Engineering (PSE) Division; Chemical Engineering Program; KAUST Catalysis Center (KCC)

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