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Charge-separation driven mechanism via acylium ion intermediate migration during catalytic carbonylation in mordenite zeolite

Author

Listed:
  • Wei Chen

    (Chinese Academy of Sciences)

  • Karolina A. Tarach

    (Jagiellonian University in Krakow)

  • Xianfeng Yi

    (Chinese Academy of Sciences)

  • Zhiqiang Liu

    (Chinese Academy of Sciences)

  • Xiaomin Tang

    (Chinese Academy of Sciences)

  • Kinga Góra-Marek

    (Jagiellonian University in Krakow)

  • Anmin Zheng

    (Chinese Academy of Sciences
    University of Chinese Academy of Sciences)

Abstract

By employing ab initio molecular dynamic simulations, solid-state NMR spectroscopy, and two-dimensional correlation analysis of rapid scan Fourier transform infrared spectroscopy data, a new pathway is proposed for the formation of methyl acetate (MA) via the acylium ion (i.e.,CH3 − C ≡ O+) in 12-membered ring (MR) channel of mordenite by an integrated reaction/diffusion kinetics model, and this route is kinetically and thermodynamically more favorable than the traditional viewpoint in 8MR channel. From perspective of the complete catalytic cycle, the separation of these two reaction zones, i.e., the C-C bond coupling in 8MR channel and MA formation in 12MR channel, effectively avoids aggregation of highly active acetyl species or ketene, thereby reducing undesired carbon deposit production. The synergistic effect of different channels appears to account for the high carbonylation activity in mordenite that has thus far not been fully explained, and this paradigm may rationalize the observed catalytic activity of other reactions.

Suggested Citation

  • 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.
    • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-34708-5
    DOI: 10.1038/s41467-022-34708-5
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    1. 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.
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