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Atomic-scale engineering of indium oxide promotion by palladium for methanol production via CO2 hydrogenation

Author

Listed:
  • Matthias S. Frei

    (ETH Zurich)

  • Cecilia Mondelli

    (ETH Zurich)

  • Rodrigo García-Muelas

    (Institute of Chemical Research of Catalonia (ICIQ), The Barcelona Institute of Science and Technology)

  • Klara S. Kley

    (ETH Zurich)

  • Begoña Puértolas

    (ETH Zurich)

  • Núria López

    (Institute of Chemical Research of Catalonia (ICIQ), The Barcelona Institute of Science and Technology)

  • Olga V. Safonova

    (Paul Scherrer Institute)

  • Joseph A. Stewart

    (Zone Industrielle Feluy C)

  • Daniel Curulla Ferré

    (Zone Industrielle Feluy C)

  • Javier Pérez-Ramírez

    (ETH Zurich)

Abstract

Metal promotion is broadly applied to enhance the performance of heterogeneous catalysts to fulfill industrial requirements. Still, generating and quantifying the effect of the promoter speciation that exclusively introduces desired properties and ensures proximity to or accommodation within the active site and durability upon reaction is very challenging. Recently, In2O3 was discovered as a highly selective and stable catalyst for green methanol production from CO2. Activity boosting by promotion with palladium, an efficient H2-splitter, was partially successful since palladium nanoparticles mediate the parasitic reverse water–gas shift reaction, reducing selectivity, and sinter or alloy with indium, limiting metal utilization and robustness. Here, we show that the precise palladium atoms architecture reached by controlled co-precipitation eliminates these limitations. Palladium atoms replacing indium atoms in the active In3O5 ensemble attract additional palladium atoms deposited onto the surface forming low-nuclearity clusters, which foster H2 activation and remain unaltered, enabling record productivities for 500 h.

Suggested Citation

  • 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.
  • Handle: RePEc:nat:natcom:v:10:y:2019:i:1:d:10.1038_s41467-019-11349-9
    DOI: 10.1038/s41467-019-11349-9
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    Cited by:

    1. 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.
    2. Thaylan Pinheiro Araújo & Georgios Giannakakis & Jordi Morales-Vidal & Mikhail Agrachev & Zaira Ruiz-Bernal & Phil Preikschas & Tangsheng Zou & Frank Krumeich & Patrik O. Willi & Wendelin J. Stark & R, 2024. "Low-nuclearity CuZn ensembles on ZnZrOx catalyze methanol synthesis from CO2," Nature Communications, Nature, vol. 15(1), pages 1-15, December.
    3. Philipp Keller & Michael A. Reiter & Patrick Kiefer & Thomas Gassler & Lucas Hemmerle & Philipp Christen & Elad Noor & Julia A. Vorholt, 2022. "Generation of an Escherichia coli strain growing on methanol via the ribulose monophosphate cycle," Nature Communications, Nature, vol. 13(1), pages 1-13, December.

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