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The role of manganese in CoMnOx catalysts for selective long-chain hydrocarbon production via Fischer-Tropsch synthesis

Author

Listed:
  • Hao Chen

    (Lawrence Berkeley National Laboratory)

  • Zan Lian

    (Barcelona Institute of Science and Technology (BIST))

  • Xiao Zhao

    (Lawrence Berkeley National Laboratory
    University of California)

  • Jiawei Wan

    (Lawrence Berkeley National Laboratory
    University of California)

  • Priscilla F. Pieters

    (University of California)

  • Judit Oliver-Meseguer

    (Lawrence Berkeley National Laboratory)

  • Ji Yang

    (Lawrence Berkeley National Laboratory)

  • Elzbieta Pach

    (Lawrence Berkeley National Laboratory)

  • Sophie Carenco

    (Lawrence Berkeley National Laboratory)

  • Laureline Treps

    (Lawrence Berkeley National Laboratory)

  • Nikos Liakakos

    (Lawrence Berkeley National Laboratory)

  • Yu Shan

    (Lawrence Berkeley National Laboratory
    University of California)

  • Virginia Altoe

    (Lawrence Berkeley National Laboratory)

  • Ed Wong

    (Lawrence Berkeley National Laboratory)

  • Zengqing Zhuo

    (Lawrence Berkeley National Laboratory)

  • Feipeng Yang

    (Lawrence Berkeley National Laboratory)

  • Ji Su

    (Lawrence Berkeley National Laboratory)

  • Jinghua Guo

    (Lawrence Berkeley National Laboratory)

  • Monika Blum

    (Lawrence Berkeley National Laboratory)

  • Saul H. Lapidus

    (Argonne National Laboratory)

  • Adrian Hunt

    (Brookhaven National Laboratory)

  • Iradwikanari Waluyo

    (Brookhaven National Laboratory)

  • Hirohito Ogasawara

    (SLAC National Accelerator Laboratory)

  • Haimei Zheng

    (Lawrence Berkeley National Laboratory
    University of California)

  • Peidong Yang

    (Lawrence Berkeley National Laboratory
    University of California
    University of California)

  • Alexis T. Bell

    (Lawrence Berkeley National Laboratory
    University of California)

  • Núria López

    (Barcelona Institute of Science and Technology (BIST))

  • Miquel Salmeron

    (Lawrence Berkeley National Laboratory
    Lawrence Berkeley National Laboratory
    University of California)

Abstract

Cobalt is an efficient catalyst for Fischer−Tropsch synthesis (FTS) of hydrocarbons from syngas (CO + H2) with enhanced selectivity for long-chain hydrocarbons when promoted by Manganese. However, the molecular scale origin of the enhancement remains unclear. Here we present an experimental and theoretical study using model catalysts consisting of crystalline CoMnOx nanoparticles and thin films, where Co and Mn are mixed at the sub-nm scale. Employing TEM and in-situ X-ray spectroscopies (XRD, APXPS, and XAS), we determine the catalyst’s atomic structure, chemical state, reactive species, and their evolution under FTS conditions. We show the concentration of CHx, the key intermediates, increases rapidly on CoMnOx, while no increase occurs without Mn. DFT simulations reveal that basic O sites in CoMnOx bind hydrogen atoms resulting from H2 dissociation on Co0 sites, making them less available to react with CHx intermediates, thus hindering chain termination reactions, which promotes the formation of long-chain hydrocarbons.

Suggested Citation

  • Hao Chen & Zan Lian & Xiao Zhao & Jiawei Wan & Priscilla F. Pieters & Judit Oliver-Meseguer & Ji Yang & Elzbieta Pach & Sophie Carenco & Laureline Treps & Nikos Liakakos & Yu Shan & Virginia Altoe & E, 2024. "The role of manganese in CoMnOx catalysts for selective long-chain hydrocarbon production via Fischer-Tropsch synthesis," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-54578-3
    DOI: 10.1038/s41467-024-54578-3
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    References listed on IDEAS

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    1. Liangshu Zhong & Fei Yu & Yunlei An & Yonghui Zhao & Yuhan Sun & Zhengjia Li & Tiejun Lin & Yanjun Lin & Xingzhen Qi & Yuanyuan Dai & Lin Gu & Jinsong Hu & Shifeng Jin & Qun Shen & Hui Wang, 2016. "Cobalt carbide nanoprisms for direct production of lower olefins from syngas," Nature, Nature, vol. 538(7623), pages 84-87, October.
    2. Yizhi Xiang & Libor Kovarik & Norbert Kruse, 2019. "Rate and selectivity hysteresis during the carbon monoxide hydrogenation over promoted Co/MnOx catalysts," Nature Communications, Nature, vol. 10(1), pages 1-7, December.
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