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Anchoring PdOx clusters on defective alumina for improved catalytic methane oxidation

Author

Listed:
  • Xiang Yu

    (Utrecht University, Universiteitsweg 99)

  • Nina S. Genz

    (Utrecht University, Universiteitsweg 99
    Forschungsstrasse 111)

  • Rafael G. Mendes

    (Utrecht University, Princetonplein 5
    1b rue de la Férollerie)

  • Xinwei Ye

    (Utrecht University, Universiteitsweg 99)

  • Florian Meirer

    (Utrecht University, Universiteitsweg 99)

  • Maarten Nachtegaal

    (Forschungsstrasse 111)

  • Matteo Monai

    (Utrecht University, Universiteitsweg 99)

  • Bert M. Weckhuysen

    (Utrecht University, Universiteitsweg 99)

Abstract

Evolution of the Pd active centers in size and spatial distribution leads to an irreversible deactivation in many high-temperature catalytic processes. This research demonstrates the use of a defective alumina (Al2O3-x) as catalyst support to anchor Pd atoms and suppress the growth of Pd clusters in catalytic methane oxidation. A combination of operando spectroscopy and density functional theory (DFT) calculations provide insights into the evolution of Pd species and reveals distinct catalytic methane oxidation mechanisms on Pd single atoms, clusters, and nanoparticles (NPs). Among these Pd species, the cluster active centers are found to be the most favorable participants in methane oxidation due to their high dispersion, high content of Pd2+ oxidation state, and resistance to deactivation by carbonates, bicarbonates, and water. The Pd/Al2O3-x catalyst shows increased stability with respect to a Pd/Al2O3 counterpart during simulated aging in alternating reducing and oxidizing conditions due to stronger interactions with the support. This study demonstrates that defect engineering of non-reducible supports can constrain the evolution of active centers, which holds promising potential for widespread utilization across diverse industrial catalytic processes, including various hydrogenation and oxidation reactions.

Suggested Citation

  • Xiang Yu & Nina S. Genz & Rafael G. Mendes & Xinwei Ye & Florian Meirer & Maarten Nachtegaal & Matteo Monai & Bert M. Weckhuysen, 2024. "Anchoring PdOx clusters on defective alumina for improved catalytic methane oxidation," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-50216-0
    DOI: 10.1038/s41467-024-50216-0
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    References listed on IDEAS

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    1. Andrey J. Zarur & Jackie Y. Ying, 2000. "Reverse microemulsion synthesis of nanostructured complex oxides for catalytic combustion," Nature, Nature, vol. 403(6765), pages 65-67, January.
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