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Operando high-pressure investigation of size-controlled CuZn catalysts for the methanol synthesis reaction

Author

Listed:
  • Núria J. Divins

    (Ruhr University Bochum
    Universitat Politècnica de Catalunya, EEBE)

  • David Kordus

    (Ruhr University Bochum
    Fritz-Haber Institute of the Max Planck Society)

  • Janis Timoshenko

    (Fritz-Haber Institute of the Max Planck Society)

  • Ilya Sinev

    (Ruhr University Bochum)

  • Ioannis Zegkinoglou

    (Ruhr University Bochum)

  • Arno Bergmann

    (Fritz-Haber Institute of the Max Planck Society)

  • See Wee Chee

    (Fritz-Haber Institute of the Max Planck Society)

  • Simon Widrinna

    (Ruhr University Bochum
    Fritz-Haber Institute of the Max Planck Society)

  • Osman Karslıoğlu

    (Fritz-Haber Institute of the Max Planck Society)

  • Hemma Mistry

    (Ruhr University Bochum)

  • Mauricio Lopez Luna

    (Fritz-Haber Institute of the Max Planck Society)

  • Jian Qiang Zhong

    (Fritz-Haber Institute of the Max Planck Society)

  • Adam S. Hoffman

    (Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory)

  • Alexey Boubnov

    (Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory)

  • J. Anibal Boscoboinik

    (Center for Functional Nanomaterials, Brookhaven National Laboratory, Upton)

  • Marc Heggen

    (Forschungszentrum Jülich)

  • Rafal E. Dunin-Borkowski

    (Forschungszentrum Jülich)

  • Simon R. Bare

    (Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory)

  • Beatriz Roldan Cuenya

    (Fritz-Haber Institute of the Max Planck Society)

Abstract

Although Cu/ZnO-based catalysts have been long used for the hydrogenation of CO2 to methanol, open questions still remain regarding the role and the dynamic nature of the active sites formed at the metal-oxide interface. Here, we apply high-pressure operando spectroscopy methods to well-defined Cu and Cu0.7Zn0.3 nanoparticles supported on ZnO/Al2O3, γ-Al2O3 and SiO2 to correlate their structure, composition and catalytic performance. We obtain similar activity and methanol selectivity for Cu/ZnO/Al2O3 and CuZn/SiO2, but the methanol yield decreases with time on stream for the latter sample. Operando X-ray absorption spectroscopy data reveal the formation of reduced Zn species coexisting with ZnO on CuZn/SiO2. Near-ambient pressure X-ray photoelectron spectroscopy shows Zn surface segregation and the formation of a ZnO-rich shell on CuZn/SiO2. In this work we demonstrate the beneficial effect of Zn, even in diluted form, and highlight the influence of the oxide support and the Cu-Zn interface in the reactivity.

Suggested Citation

  • Núria J. Divins & David Kordus & Janis Timoshenko & Ilya Sinev & Ioannis Zegkinoglou & Arno Bergmann & See Wee Chee & Simon Widrinna & Osman Karslıoğlu & Hemma Mistry & Mauricio Lopez Luna & Jian Qian, 2021. "Operando high-pressure investigation of size-controlled CuZn catalysts for the methanol synthesis reaction," Nature Communications, Nature, vol. 12(1), pages 1-10, December.
    • Handle: RePEc:nat:natcom:v:12:y:2021:i:1:d:10.1038_s41467-021-21604-7
    DOI: 10.1038/s41467-021-21604-7
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    Cited by:

    1. Hao Meng & Yusen Yang & Tianyao Shen & Zhiming Yin & Lei Wang & Wei Liu & Pan Yin & Zhen Ren & Lirong Zheng & Jian Zhang & Feng-Shou Xiao & Min Wei, 2023. "Designing Cu0−Cu+ dual sites for improved C−H bond fracture towards methanol steam reforming," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    2. Sigmund Jensen & Mathias H. R. Mammen & Martin Hedevang & Zheshen Li & Lutz Lammich & Jeppe V. Lauritsen, 2024. "Visualizing the gas-sensitive structure of the CuZn surface in methanol synthesis catalysis," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    3. Runping Ye & Lixuan Ma & Jianing Mao & Xinyao Wang & Xiaoling Hong & Alessandro Gallo & Yanfu Ma & Wenhao Luo & Baojun Wang & Riguang Zhang & Melis Seher Duyar & Zheng Jiang & Jian Liu, 2024. "A Ce-CuZn catalyst with abundant Cu/Zn-OV-Ce active sites for CO2 hydrogenation to methanol," Nature Communications, Nature, vol. 15(1), pages 1-14, December.
    4. Núria. J. Divins & Andrea Braga & Xavier Vendrell & Isabel Serrano & Xènia Garcia & Lluís Soler & Ilaria Lucentini & Maila Danielis & Andrea Mussio & Sara Colussi & Ignacio J. Villar-Garcia & Carlos E, 2022. "Investigation of the evolution of Pd-Pt supported on ceria for dry and wet methane oxidation," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
    5. Si Woo Lee & Mauricio Lopez Luna & Nikolay Berdunov & Weiming Wan & Sebastian Kunze & Shamil Shaikhutdinov & Beatriz Roldan Cuenya, 2023. "Unraveling surface structures of gallium promoted transition metal catalysts in CO2 hydrogenation," Nature Communications, Nature, vol. 14(1), pages 1-7, December.

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