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Real-time insight into the multistage mechanism of nanoparticle exsolution from a perovskite host surface

Author

Listed:
  • Eleonora Calì

    (Imperial College London
    Politecnico di Torino)

  • Melonie P. Thomas

    (University of Kentucky
    University of Peradeniya)

  • Rama Vasudevan

    (Oak Ridge National Laboratory)

  • Ji Wu

    (University of Bath
    Queen Mary University of London)

  • Oriol Gavalda-Diaz

    (Imperial College London
    The University of Nottingham)

  • Katharina Marquardt

    (Imperial College London)

  • Eduardo Saiz

    (Imperial College London)

  • Dragos Neagu

    (University of Strathclyde)

  • Raymond R. Unocic

    (Oak Ridge National Laboratory)

  • Stephen C. Parker

    (University of Bath)

  • Beth S. Guiton

    (University of Kentucky)

  • David J. Payne

    (Imperial College London
    Harwell Science and Innovation Campus)

Abstract

In exsolution, nanoparticles form by emerging from oxide hosts by application of redox driving forces, leading to transformative advances in stability, activity, and efficiency over deposition techniques, and resulting in a wide range of new opportunities for catalytic, energy and net-zero-related technologies. However, the mechanism of exsolved nanoparticle nucleation and perovskite structural evolution, has, to date, remained unclear. Herein, we shed light on this elusive process by following in real time Ir nanoparticle emergence from a SrTiO3 host oxide lattice, using in situ high-resolution electron microscopy in combination with computational simulations and machine learning analytics. We show that nucleation occurs via atom clustering, in tandem with host evolution, revealing the participation of surface defects and host lattice restructuring in trapping Ir atoms to initiate nanoparticle formation and growth. These insights provide a theoretical platform and practical recommendations to further the development of highly functional and broadly applicable exsolvable materials.

Suggested Citation

  • Eleonora Calì & Melonie P. Thomas & Rama Vasudevan & Ji Wu & Oriol Gavalda-Diaz & Katharina Marquardt & Eduardo Saiz & Dragos Neagu & Raymond R. Unocic & Stephen C. Parker & Beth S. Guiton & David J. , 2023. "Real-time insight into the multistage mechanism of nanoparticle exsolution from a perovskite host surface," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-37212-6
    DOI: 10.1038/s41467-023-37212-6
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    References listed on IDEAS

    as
    1. Dragos Neagu & Tae-Sik Oh & David N. Miller & Hervé Ménard & Syed M. Bukhari & Stephen R. Gamble & Raymond J. Gorte & John M. Vohs & John T.S. Irvine, 2015. "Nano-socketed nickel particles with enhanced coking resistance grown in situ by redox exsolution," Nature Communications, Nature, vol. 6(1), pages 1-8, November.
    2. Lingting Ye & Minyi Zhang & Ping Huang & Guocong Guo & Maochun Hong & Chunsen Li & John T. S. Irvine & Kui Xie, 2017. "Enhancing CO2 electrolysis through synergistic control of non-stoichiometry and doping to tune cathode surface structures," Nature Communications, Nature, vol. 8(1), pages 1-10, April.
    3. Jae-ha Myung & Dragos Neagu & David N. Miller & John T. S. Irvine, 2016. "Switching on electrocatalytic activity in solid oxide cells," Nature, Nature, vol. 537(7621), pages 528-531, September.
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