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    Metal Organic Framework Derived Synthesis of Cobalt Indium Catalysts for the Hydrogenation of CO2 to methanol

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    Type
    Article
    Authors
    Pustovarenko, Alexey
    Dikhtiarenko, Alla
    Bavykina, Anastasiya
    Gevers, Lieven
    Ramirez, Adrian
    Russkikh, Artem
    Telalovic, Selvedin
    Aguilar, Antonio
    Hazemann, Jean Louis
    Ould-Chikh, Samy cc
    Gascon, Jorge cc
    KAUST Department
    Chemical Engineering Program
    Chemical Science
    KAUST Catalysis Center (KCC)
    King Abdullah University of Science and Technology, KAUST Catalysis Center (KCC), Advanced Catalytic Materials, Thuwal 23955, Saudi Arabia.
    Physical Science and Engineering (PSE) Division
    Date
    2020-04-03
    Online Publication Date
    2020-04-03
    Print Publication Date
    2020-05-01
    Embargo End Date
    2021-04-03
    Permanent link to this record
    http://hdl.handle.net/10754/662470
    
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    Abstract
    Methanol synthesis by means of direct CO2 hydrogenation has the potential to contribute to climate change mitigation by turning the most important greenhouse gas into a commodity. However, for this process to become industrially relevant, catalytic systems with improved activity, selectivity and stability are required. Here we explore the potential of metal-organic frameworks (MOF) as precursors for synthesis of Co3O4-supported In2O3 oxide composites for the direct CO2 hydrogenation to methanol. Stepwise pyrolytic-oxidative decomposition of indium-impregnated ZIF-67(Co) MOF affords the formation of a nanostructured In2O3@Co3O4 reticulated shell composite material able to reach a maximum methanol production rate of 0.65 gMeOH·gcat-1·h-1 with selectivity as high as 87% over 100 h on stream. Textural characteristics of the sacrificial ZIF-67(Co) matrix and In-loading were found to be important variables for optimizing the catalyst performance such as induction time, methanol productivity and selectivity. The structural investigation on the catalytic system reveals that the catalyst undergoes reorganization under reaction conditions, transforming from a Co3O4 with amorphous In2O3 shell into Co3InC0.75 covered by a layer consisting of a mixture of amorphous CoOx and In2O3 oxides. Structural reorganization is responsible for the observed induction period, while the amorphous mixed cobalt indium oxide shell is responsible for the high methanol yield and selectivity. Additionally, these results demonstrate the tunable performance of MOF-derived In2O3@Co3O4 catalyst as a function of the reaction conditions which allows to establish a reasonable trade-off between high methanol yield and selectivity in a wide temperature and pressure window.
    Citation
    Pustovarenko, A., Dikhtiarenko, A., Bavykina, A., Gevers, L. E., Ramirez, A., Russkikh, A., … Gascon, J. (2020). Metal Organic Framework Derived Synthesis of Cobalt Indium Catalysts for the Hydrogenation of CO2 to methanol. ACS Catalysis. doi:10.1021/acscatal.0c00449
    Sponsors
    The authors gratefully acknowledge the European Synchrotron Radiation Facility (Grenoble, France) for provision of beamtime (CH 5572) for XAS experiments carried out on the FAME beamline (BM30B) and support of their staff.
    Funding for this work was provided by King Abdullah University of Science and Technology (KAUST).
    Publisher
    American Chemical Society (ACS)
    Journal
    ACS Catalysis
    DOI
    10.1021/acscatal.0c00449
    Additional Links
    https://pubs.acs.org/doi/10.1021/acscatal.0c00449
    ae974a485f413a2113503eed53cd6c53
    10.1021/acscatal.0c00449
    Scopus Count
    Collections
    Articles; Physical Science and Engineering (PSE) Division; Chemical Engineering Program; KAUST Catalysis Center (KCC)

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