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Directing reaction pathways via in situ control of active site geometries in PdAu single-atom alloy catalysts

Author

Listed:
  • Mengyao Ouyang

    (Tufts University)

  • Konstantinos G. Papanikolaou

    (University College London)

  • Alexey Boubnov

    (SLAC National Accelerator Laboratory)

  • Adam S. Hoffman

    (SLAC National Accelerator Laboratory)

  • Georgios Giannakakis

    (Tufts University)

  • Simon R. Bare

    (SLAC National Accelerator Laboratory)

  • Michail Stamatakis

    (University College London)

  • Maria Flytzani-Stephanopoulos

    (Tufts University)

  • E. Charles H. Sykes

    (Tufts University)

Abstract

The atomic scale structure of the active sites in heterogeneous catalysts is central to their reactivity and selectivity. Therefore, understanding active site stability and evolution under different reaction conditions is key to the design of efficient and robust catalysts. Herein we describe theoretical calculations which predict that carbon monoxide can be used to stabilize different active site geometries in bimetallic alloys and then demonstrate experimentally that the same PdAu bimetallic catalyst can be transitioned between a single-atom alloy and a Pd cluster phase. Each state of the catalyst exhibits distinct selectivity for the dehydrogenation of ethanol reaction with the single-atom alloy phase exhibiting high selectivity to acetaldehyde and hydrogen versus a range of products from Pd clusters. First-principles based Monte Carlo calculations explain the origin of this active site ensemble size tuning effect, and this work serves as a demonstration of what should be a general phenomenon that enables in situ control over catalyst selectivity.

Suggested Citation

  • Mengyao Ouyang & Konstantinos G. Papanikolaou & Alexey Boubnov & Adam S. Hoffman & Georgios Giannakakis & Simon R. Bare & Michail Stamatakis & Maria Flytzani-Stephanopoulos & E. Charles H. Sykes, 2021. "Directing reaction pathways via in situ control of active site geometries in PdAu single-atom alloy catalysts," Nature Communications, Nature, vol. 12(1), pages 1-11, December.
    • Handle: RePEc:nat:natcom:v:12:y:2021:i:1:d:10.1038_s41467-021-21555-z
    DOI: 10.1038/s41467-021-21555-z
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    Cited by:

    1. Chen, Zhangsen & Zhang, Gaixia & Chen, Hangrong & Prakash, Jai & Zheng, Yi & Sun, Shuhui, 2022. "Multi-metallic catalysts for the electroreduction of carbon dioxide: Recent advances and perspectives," Renewable and Sustainable Energy Reviews, Elsevier, vol. 155(C).
    2. Wei Liu & Haisong Feng & Yusen Yang & Yiming Niu & Lei Wang & Pan Yin & Song Hong & Bingsen Zhang & Xin Zhang & Min Wei, 2022. "Highly-efficient RuNi single-atom alloy catalysts toward chemoselective hydrogenation of nitroarenes," Nature Communications, Nature, vol. 13(1), pages 1-12, December.
    3. Chengxin Zhou & Jian Gao & Yunlong Deng & Ming Wang & Dan Li & Chuan Xia, 2023. "Electric double layer-mediated polarization field for optimizing photogenerated carrier dynamics and thermodynamics," Nature Communications, Nature, vol. 14(1), pages 1-11, December.

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