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The unique interplay between copper and zinc during catalytic carbon dioxide hydrogenation to methanol

Author

Listed:
  • Maxim Zabilskiy

    (Paul Scherrer Institute)

  • Vitaly L. Sushkevich

    (Paul Scherrer Institute)

  • Dennis Palagin

    (Paul Scherrer Institute)

  • Mark A. Newton

    (ETH Zurich)

  • Frank Krumeich

    (ETH Zurich)

  • Jeroen A. Bokhoven

    (Paul Scherrer Institute
    ETH Zurich)

Abstract

In spite of numerous works in the field of chemical valorization of carbon dioxide into methanol, the nature of high activity of Cu/ZnO catalysts, including the reaction mechanism and the structure of the catalyst active site, remains the subject of intensive debate. By using high-pressure operando techniques: steady-state isotope transient kinetic analysis coupled with infrared spectroscopy, together with time-resolved X-ray absorption spectroscopy and X-ray powder diffraction, and supported by electron microscopy and theoretical modeling, we present direct evidence that zinc formate is the principal observable reactive intermediate, which in the presence of hydrogen converts into methanol. Our results indicate that the copper–zinc alloy undergoes oxidation under reaction conditions into zinc formate, zinc oxide and metallic copper. The intimate contact between zinc and copper phases facilitates zinc formate formation and its hydrogenation by hydrogen to methanol.

Suggested Citation

  • Maxim Zabilskiy & Vitaly L. Sushkevich & Dennis Palagin & Mark A. Newton & Frank Krumeich & Jeroen A. Bokhoven, 2020. "The unique interplay between copper and zinc during catalytic carbon dioxide hydrogenation to methanol," Nature Communications, Nature, vol. 11(1), pages 1-8, December.
    • Handle: RePEc:nat:natcom:v:11:y:2020:i:1:d:10.1038_s41467-020-16342-1
    DOI: 10.1038/s41467-020-16342-1
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    Cited by:

    1. Guo Tian & Zhengwen Li & Chenxi Zhang & Xinyan Liu & Xiaoyu Fan & Kui Shen & Haibin Meng & Ning Wang & Hao Xiong & Mingyu Zhao & Xiaoyu Liang & Liqiang Luo & Lan Zhang & Binhang Yan & Xiao Chen & Hong, 2024. "Upgrading CO2 to sustainable aromatics via perovskite-mediated tandem catalysis," Nature Communications, Nature, vol. 15(1), pages 1-13, December.
    2. Han, Jian & Yu, Jun & Xue, Zhaoteng & Wu, Guisheng & Mao, Dongsen, 2024. "Highly efficient CO2 hydrogenation to methanol over Cu–Ce1-xZrxO2 catalysts prepared by an eco-friendly and facile solid-phase grinding method," Renewable Energy, Elsevier, vol. 222(C).
    3. 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.
    4. 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.

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