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Flame-made ternary Pd-In2O3-ZrO2 catalyst with enhanced oxygen vacancy generation for CO2 hydrogenation to methanol

Author

Listed:
  • Thaylan Pinheiro Araújo

    (Institute of Chemical and Bioengineering, Department of Chemistry and Applied Biosciences, ETH Zurich)

  • Cecilia Mondelli

    (Institute of Chemical and Bioengineering, Department of Chemistry and Applied Biosciences, ETH Zurich)

  • Mikhail Agrachev

    (Laboratory of Physical Chemistry, Department of Chemistry and Applied Biosciences, ETH Zurich)

  • Tangsheng Zou

    (Institute of Chemical and Bioengineering, Department of Chemistry and Applied Biosciences, ETH Zurich)

  • Patrik O. Willi

    (Institute of Chemical and Bioengineering, Department of Chemistry and Applied Biosciences, ETH Zurich)

  • Konstantin M. Engel

    (Institute of Chemical and Bioengineering, Department of Chemistry and Applied Biosciences, ETH Zurich)

  • Robert N. Grass

    (Institute of Chemical and Bioengineering, Department of Chemistry and Applied Biosciences, ETH Zurich)

  • Wendelin J. Stark

    (Institute of Chemical and Bioengineering, Department of Chemistry and Applied Biosciences, ETH Zurich)

  • Olga V. Safonova

    (Paul Scherrer Institute)

  • Gunnar Jeschke

    (Laboratory of Physical Chemistry, Department of Chemistry and Applied Biosciences, ETH Zurich)

  • Sharon Mitchell

    (Institute of Chemical and Bioengineering, Department of Chemistry and Applied Biosciences, ETH Zurich)

  • Javier Pérez-Ramírez

    (Institute of Chemical and Bioengineering, Department of Chemistry and Applied Biosciences, ETH Zurich)

Abstract

Palladium promotion and deposition on monoclinic zirconia are effective strategies to boost the performance of bulk In2O3 in CO2-to-methanol and could unlock superior reactivity if well integrated into a single catalytic system. However, harnessing synergic effects of the individual components is crucial and very challenging as it requires precise control over their assembly. Herein, we present ternary Pd-In2O3-ZrO2 catalysts prepared by flame spray pyrolysis (FSP) with remarkable methanol productivity and improved metal utilization, surpassing their binary counterparts. Unlike established impregnation and co-precipitation methods, FSP produces materials combining low-nuclearity palladium species associated with In2O3 monolayers highly dispersed on the ZrO2 carrier, whose surface partially transforms from a tetragonal into a monoclinic-like structure upon reaction. A pioneering protocol developed to quantify oxygen vacancies using in situ electron paramagnetic resonance spectroscopy reveals their enhanced generation because of this unique catalyst architecture, thereby rationalizing its high and sustained methanol productivity.

Suggested Citation

  • Thaylan Pinheiro Araújo & Cecilia Mondelli & Mikhail Agrachev & Tangsheng Zou & Patrik O. Willi & Konstantin M. Engel & Robert N. Grass & Wendelin J. Stark & Olga V. Safonova & Gunnar Jeschke & Sharon, 2022. "Flame-made ternary Pd-In2O3-ZrO2 catalyst with enhanced oxygen vacancy generation for CO2 hydrogenation to methanol," Nature Communications, Nature, vol. 13(1), pages 1-12, December.
    • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-33391-w
    DOI: 10.1038/s41467-022-33391-w
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    References listed on IDEAS

    as
    1. Matthias S. Frei & Cecilia Mondelli & Rodrigo García-Muelas & Klara S. Kley & Begoña Puértolas & Núria López & Olga V. Safonova & Joseph A. Stewart & Daniel Curulla Ferré & Javier Pérez-Ramírez, 2019. "Atomic-scale engineering of indium oxide promotion by palladium for methanol production via CO2 hydrogenation," Nature Communications, Nature, vol. 10(1), pages 1-11, December.
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    Cited by:

    1. 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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