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Exploiting two-dimensional morphology of molybdenum oxycarbide to enable efficient catalytic dry reforming of methane

Author

Listed:
  • Alexey Kurlov

    (ETH Zürich)

  • Evgeniya B. Deeva

    (ETH Zürich)

  • Paula M. Abdala

    (ETH Zürich)

  • Dmitry Lebedev

    (ETH Zürich
    Northwestern University)

  • Athanasia Tsoukalou

    (ETH Zürich)

  • Aleix Comas-Vives

    (Universitat Autònoma de Barcelona)

  • Alexey Fedorov

    (ETH Zürich)

  • Christoph R. Müller

    (ETH Zürich)

Abstract

The two-dimensional morphology of molybdenum oxycarbide (2D-Mo2COx) nanosheets dispersed on silica is found vital for imparting high stability and catalytic activity in the dry reforming of methane. Here we report that owing to the maximized metal utilization, the specific activity of 2D-Mo2COx/SiO2 exceeds that of other Mo2C catalysts by ca. 3 orders of magnitude. 2D-Mo2COx is activated by CO2, yielding a surface oxygen coverage that is optimal for its catalytic performance and a Mo oxidation state of ca. +4. According to ab initio calculations, the DRM proceeds on Mo sites of the oxycarbide nanosheet with an oxygen coverage of 0.67 monolayer. Methane activation is the rate-limiting step, while the activation of CO2 and the C–O coupling to form CO are low energy steps. The deactivation of 2D-Mo2COx/SiO2 under DRM conditions can be avoided by tuning the contact time, thereby preventing unfavourable oxygen surface coverages.

Suggested Citation

  • Alexey Kurlov & Evgeniya B. Deeva & Paula M. Abdala & Dmitry Lebedev & Athanasia Tsoukalou & Aleix Comas-Vives & Alexey Fedorov & Christoph R. Müller, 2020. "Exploiting two-dimensional morphology of molybdenum oxycarbide to enable efficient catalytic dry reforming of methane," Nature Communications, Nature, vol. 11(1), pages 1-11, December.
    • Handle: RePEc:nat:natcom:v:11:y:2020:i:1:d:10.1038_s41467-020-18721-0
    DOI: 10.1038/s41467-020-18721-0
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    Cited by:

    1. Bian, Zhoufeng & Deng, Shaobi & Sun, Zhenkun & Ge, Tianshu & Jiang, Bo & Zhong, Wenqi, 2022. "Multi-core@Shell catalyst derived from LDH@SiO2 for low- temperature dry reforming of methane," Renewable Energy, Elsevier, vol. 200(C), pages 1362-1370.
    2. Bin Shao & Zhi-Qiang Wang & Xue-Qing Gong & Honglai Liu & Feng Qian & P. Hu & Jun Hu, 2023. "Synergistic promotions between CO2 capture and in-situ conversion on Ni-CaO composite catalyst," Nature Communications, Nature, vol. 14(1), pages 1-10, December.

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