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Designing main-group catalysts for low-temperature methane combustion by ozone

Author

Listed:
  • Shunsaku Yasumura

    (Hokkaido University)

  • Kenichiro Saita

    (Hokkaido University)

  • Takumi Miyakage

    (Hokkaido University)

  • Ken Nagai

    (Hokkaido University)

  • Kenichi Kon

    (Hokkaido University)

  • Takashi Toyao

    (Hokkaido University)

  • Zen Maeno

    (Kogakuin University)

  • Tetsuya Taketsugu

    (Hokkaido University
    Hokkaido University)

  • Ken-ichi Shimizu

    (Hokkaido University)

Abstract

The catalytic combustion of methane at a low temperature is becoming increasingly key to controlling unburned CH4 emissions from natural gas vehicles and power plants, although the low activity of benchmark platinum-group-metal catalysts hinders its broad application. Based on automated reaction route mapping, we explore main-group elements catalysts containing Si and Al for low-temperature CH4 combustion with ozone. Computational screening of the active site predicts that strong Brønsted acid sites are promising for methane combustion. We experimentally demonstrate that catalysts containing strong Bronsted acid sites exhibit improved CH4 conversion at 250 °C, correlating with the theoretical predictions. The main-group catalyst (proton-type beta zeolite) delivered a reaction rate that is 442 times higher than that of a benchmark catalyst (5 wt% Pd-loaded Al2O3) at 190 °C and exhibits higher tolerance to steam and SO2. Our strategy demonstrates the rational design of earth-abundant catalysts based on automated reaction route mapping.

Suggested Citation

  • Shunsaku Yasumura & Kenichiro Saita & Takumi Miyakage & Ken Nagai & Kenichi Kon & Takashi Toyao & Zen Maeno & Tetsuya Taketsugu & Ken-ichi Shimizu, 2023. "Designing main-group catalysts for low-temperature methane combustion by ozone," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-39541-y
    DOI: 10.1038/s41467-023-39541-y
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    References listed on IDEAS

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    1. Sina Stocker & Gábor Csányi & Karsten Reuter & Johannes T. Margraf, 2020. "Machine learning in chemical reaction space," Nature Communications, Nature, vol. 11(1), pages 1-11, December.
    2. Andrey W. Petrov & Davide Ferri & Frank Krumeich & Maarten Nachtegaal & Jeroen A. van Bokhoven & Oliver Kröcher, 2018. "Stable complete methane oxidation over palladium based zeolite catalysts," Nature Communications, Nature, vol. 9(1), pages 1-8, December.
    3. Zachary W. Ulissi & Andrew J. Medford & Thomas Bligaard & Jens K. Nørskov, 2017. "To address surface reaction network complexity using scaling relations machine learning and DFT calculations," Nature Communications, Nature, vol. 8(1), pages 1-7, April.
    4. He, Li & Fan, Yilin & Bellettre, Jérôme & Yue, Jun & Luo, Lingai, 2020. "A review on catalytic methane combustion at low temperatures: Catalysts, mechanisms, reaction conditions and reactor designs," Renewable and Sustainable Energy Reviews, Elsevier, vol. 119(C).
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