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Selectivity descriptors for the direct hydrogenation of CO2 to hydrocarbons during zeolite-mediated bifunctional catalysis

Author

Listed:
  • Adrian Ramirez

    (King Abdullah University of Science and Technology (KAUST))

  • Xuan Gong

    (Wuhan University)

  • Mustafa Caglayan

    (King Abdullah University of Science and Technology (KAUST))

  • Stefan-Adrian F. Nastase

    (King Abdullah University of Science and Technology (KAUST))

  • Edy Abou-Hamad

    (King Abdullah University of Science and Technology (KAUST))

  • Lieven Gevers

    (King Abdullah University of Science and Technology (KAUST))

  • Luigi Cavallo

    (King Abdullah University of Science and Technology (KAUST))

  • Abhishek Dutta Chowdhury

    (Wuhan University)

  • Jorge Gascon

    (King Abdullah University of Science and Technology (KAUST))

Abstract

Cascade processes are gaining momentum in heterogeneous catalysis. The combination of several catalytic solids within one reactor has shown great promise for the one-step valorization of C1-feedstocks. The combination of metal-based catalysts and zeolites in the gas phase hydrogenation of CO2 leads to a large degree of product selectivity control, defined mainly by zeolites. However, a great deal of mechanistic understanding remains unclear: metal-based catalysts usually lead to complex product compositions that may result in unexpected zeolite reactivity. Here we present an in-depth multivariate analysis of the chemistry involved in eight different zeolite topologies when combined with a highly active Fe-based catalyst in the hydrogenation of CO2 to olefins, aromatics, and paraffins. Solid-state NMR spectroscopy and computational analysis demonstrate that the hybrid nature of the active zeolite catalyst and its preferred CO2-derived reaction intermediates (CO/ester/ketone/hydrocarbons, i.e., inorganic-organic supramolecular reactive centers), along with 10 MR-zeolite topology, act as descriptors governing the ultimate product selectivity.

Suggested Citation

  • Adrian Ramirez & Xuan Gong & Mustafa Caglayan & Stefan-Adrian F. Nastase & Edy Abou-Hamad & Lieven Gevers & Luigi Cavallo & Abhishek Dutta Chowdhury & Jorge Gascon, 2021. "Selectivity descriptors for the direct hydrogenation of CO2 to hydrocarbons during zeolite-mediated bifunctional catalysis," Nature Communications, Nature, vol. 12(1), pages 1-13, December.
    • Handle: RePEc:nat:natcom:v:12:y:2021:i:1:d:10.1038_s41467-021-26090-5
    DOI: 10.1038/s41467-021-26090-5
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    References listed on IDEAS

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    1. Youming Ni & Zhiyang Chen & Yi Fu & Yong Liu & Wenliang Zhu & Zhongmin Liu, 2018. "Selective conversion of CO2 and H2 into aromatics," Nature Communications, Nature, vol. 9(1), pages 1-7, December.
    2. Jian Wei & Qingjie Ge & Ruwei Yao & Zhiyong Wen & Chuanyan Fang & Lisheng Guo & Hengyong Xu & Jian Sun, 2017. "Directly converting CO2 into a gasoline fuel," Nature Communications, Nature, vol. 8(1), pages 1-9, August.
    3. Niall Mac Dowell & Paul S. Fennell & Nilay Shah & Geoffrey C. Maitland, 2017. "The role of CO2 capture and utilization in mitigating climate change," Nature Climate Change, Nature, vol. 7(4), pages 243-249, April.
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    Cited by:

    1. Pengfei Zhang & Viko Ladelta & Edy Abou-hamad & Alejandro J. Müller & Nikos Hadjichristidis, 2023. "Catalyst switch strategy enabled a single polymer with five different crystalline phases," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    2. Hao-Xin Liu & Wei-Wei Wang & Xin-Pu Fu & Jin-Cheng Liu & Chun-Jiang Jia, 2024. "Direct cleavage of C=O double bond in CO2 by the subnano MoOx surface on Mo2N," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    3. Wei Chen & Karolina A. Tarach & Xianfeng Yi & Zhiqiang Liu & Xiaomin Tang & Kinga Góra-Marek & Anmin Zheng, 2022. "Charge-separation driven mechanism via acylium ion intermediate migration during catalytic carbonylation in mordenite zeolite," Nature Communications, Nature, vol. 13(1), pages 1-13, December.

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