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Decisive Influence of SAPO-34 Zeolite on Light Olefin Selectivity in Methanol-Meditated CO2 Hydrogenation over Metal Oxide-Zeolite Catalysts

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    Research Article

    Decisive Influence of SAPO-34 Zeolite on Light Olefin Selectivity in Methanol-Meditated CO2 Hydrogenation over Metal Oxide-Zeolite Catalysts
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    ACS Catalysis

    Cite this: ACS Catal. 2023, 13, 22, 14627–14638
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    https://doi.org/10.1021/acscatal.3c03759
    Published October 30, 2023
    Copyright © 2023 American Chemical Society
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    Abstract

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    Methanol-mediated CO2 selective hydrogenation to light olefins (LO) over bifunctional catalysts containing metal oxide and zeolite components is an attractive sustainable chemical process. The main challenges of this process include achieving high LO selectivity and low selectivity to light paraffins and CO. Herein, we analyze the selectivity–conversion correlations over metal oxide-zeolite bifunctional catalysts and elucidate the functions of each catalyst component. A series of catalytic systems based on oxides of Zn, In, Mn, Cr, or Ga and different SAPO-34 zeolites were synthesized and evaluated at different CO2 conversion levels. It was uncovered that the selectivity to LO within hydrocarbon fractions ultimately depended on the zeolite component and decreased as a function of the hydrocarbon yield. The metal oxide catalyst component was responsible for the CO2 conversion, overall hydrocarbon, and CO selectivities. The SAPO-34 morphology and acidity were identified as major descriptors of the CO-free LO selectivity in the CO2 hydrogenation over bifunctional metal oxide-zeolite catalysts.

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acscatal.3c03759.

    • Experimental details; description of TAP experiments and data processing; phase analysis of XRD data and coherent scattering area sizes; SEM data; CO2-TPD patterns and their quantitative analysis; selectivity–conversion graphs; TAP results (PDF)

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    Cited By

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    This article is cited by 4 publications.

    1. Massimo Corda, Sergei A. Chernyak, Maya Marinova, Jean-Charles Morin, Martine Trentesaux, Vita A. Kondratenko, Evgenii V. Kondratenko, Vitaly V. Ordomsky, Andrei Y. Khodakov. Selective CO2 Hydrogenation to Methanol by Halogen Deposition over a Cu-Based Catalyst. ACS Catalysis 2024, 14 (23) , 17244-17252. https://doi.org/10.1021/acscatal.4c04824
    2. Qingxin Yang, Evgenii V. Kondratenko. From Understanding of Catalyst Functioning toward Controlling Selectivity in CO2 Hydrogenation to Higher Hydrocarbons over Fe-Based Catalysts. Accounts of Materials Research 2024, 5 (11) , 1314-1328. https://doi.org/10.1021/accountsmr.4c00160
    3. Foteini Lappa, Ibrahim Khalil, Alejandro Morales, Grégoire Léonard, Michiel Dusselier. One Step Methanol-Mediated CO2 Conversion to Gasoline: Comprehensive Review and Critical Outlook. Energy & Fuels 2024, 38 (19) , 18265-18291. https://doi.org/10.1021/acs.energyfuels.4c03013
    4. Kang Cheng, Yubing Li, Jincan Kang, Qinghong Zhang, Ye Wang. Selectivity Control by Relay Catalysis in CO and CO2 Hydrogenation to Multicarbon Compounds. Accounts of Chemical Research 2024, 57 (5) , 714-725. https://doi.org/10.1021/acs.accounts.3c00734
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    ACS Catalysis

    Cite this: ACS Catal. 2023, 13, 22, 14627–14638
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acscatal.3c03759
    Published October 30, 2023
    Copyright © 2023 American Chemical Society
    Request reuse permissions

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