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Nanoparticle Metamorphosis: An in Situ High-Temperature Transmission Electron Microscopy Study of the Structural Evolution of Heterogeneous Au:Fe2O3 Nanoparticles

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    Nanoparticle Metamorphosis: An in Situ High-Temperature Transmission Electron Microscopy Study of the Structural Evolution of Heterogeneous Au:Fe2O3 Nanoparticles
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    † Department of Chemical and Biomolecular Engineering, Cornell University, Ithaca, New York 14853, United States
    ‡ Department of Chemistry and Chemical Biology, Cornell University, Ithaca, New York 14853, United States
    § School of Applied Engineering and Physics, Cornell University, Ithaca, New York 14853, United States
    ∥ Department of Materials Science and Engineering, Cornell University, Ithaca, New York 14853, United States
    ⊥ Kavli Institute at Cornell for Nanoscale Science, Ithaca, New York 14853, United States
    *Address correspondence to [email protected]
    Other Access OptionsSupporting Information (4)

    ACS Nano

    Cite this: ACS Nano 2014, 8, 5, 5315–5322
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    https://doi.org/10.1021/nn501543d
    Published April 23, 2014
    Copyright © 2014 American Chemical Society
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    Abstract

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    High-temperature in situ electron microscopy and X-ray diffraction have revealed that Au and Fe2O3 particles fuse in a fluid fashion at temperatures far below their size-reduced melting points. With increasing temperature, the fused particles undergo a sequence of complex structural transformations from surface alloy to phase segregated and ultimately core–shell structures. The combination of in situ electron microscopy and spectroscopy provides insights into fundamental thermodynamic and kinetic aspects governing the formation of heterogeneous nanostructures. The observed structural transformations present an interesting analogy to thin film growth on the curved surface of a nanoparticle. Using single-particle observations, we constructed a phase diagram illustrating the complex relationships among composition, morphology, temperature, and particle size.

    Copyright © 2014 American Chemical Society

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    Supporting Information

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    Detailed information on nanoparticle synthesis, beam dosage effect, quantification of beam dose, X-ray diffraction, surface energy changes driving NP sintering, thickness of a thin film formed on the surface of an NP, DFT calculations of Au within a hematite lattice, EELS analysis, electron diffraction and atomic-resolution imaging, and movies are provided. This material is available free of charge via the Internet at http://pubs.acs.org.

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    Cited By

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    This article is cited by 11 publications.

    1. Julien Ramade, Emmanuel Cottancin, Marie-Ange Lebeault, Cyril Langlois, Laurent Piccolo, Michel Broyer, Matthias Hillenkamp, Jean Lermé, Florent Calvo, Michel Pellarin. Environmental Plasmonic Spectroscopy of Silver–Iron Nanoparticles: Chemical Ordering under Oxidizing and Reducing Conditions. The Journal of Physical Chemistry C 2019, 123 (25) , 15693-15706. https://doi.org/10.1021/acs.jpcc.9b02422
    2. Xingchen Liu, Xiaodong Wen, Roald Hoffmann. Surface Activation of Transition Metal Nanoparticles for Heterogeneous Catalysis: What We Can Learn from Molecular Dynamics. ACS Catalysis 2018, 8 (4) , 3365-3375. https://doi.org/10.1021/acscatal.7b04468
    3. Kevin Whitham and Tobias Hanrath . Formation of Epitaxially Connected Quantum Dot Solids: Nucleation and Coherent Phase Transition. The Journal of Physical Chemistry Letters 2017, 8 (12) , 2623-2628. https://doi.org/10.1021/acs.jpclett.7b00846
    4. Dang Sheng Su, Bingsen Zhang, and Robert Schlögl . Electron Microscopy of Solid Catalysts—Transforming from a Challenge to a Toolbox. Chemical Reviews 2015, 115 (8) , 2818-2882. https://doi.org/10.1021/cr500084c
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    6. D. Akcan. Effect of type and concentration of cobalt precursor on structural, optical and defect properties of ZnCoO nanoparticles. Materials Research Bulletin 2021, 139 , 111254. https://doi.org/10.1016/j.materresbull.2021.111254
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    11. Julien Ramade, Cyril Langlois, Michel Pellarin, Laurent Piccolo, Marie-Ange Lebeault, Thierry Epicier, Mimoun Aouine, Emmanuel Cottancin. Tracking the restructuring of oxidized silver–indium nanoparticles under a reducing atmosphere by environmental HRTEM. Nanoscale 2017, 9 (36) , 13563-13574. https://doi.org/10.1039/C7NR02986A
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    ACS Nano

    Cite this: ACS Nano 2014, 8, 5, 5315–5322
    Click to copy citationCitation copied!
    https://doi.org/10.1021/nn501543d
    Published April 23, 2014
    Copyright © 2014 American Chemical Society
    Request reuse permissions

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