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Real Time Monitoring of the Dynamic Intracluster Diffusion of Single Gold Atoms into Silver Nanoclusters

  • Kaiyuan Zheng
    Kaiyuan Zheng
    Department of Chemical and Biomolecular Engineering, National University of Singapore, 4 Engineering Drive 4, 117585 Singapore
    More by Kaiyuan Zheng
    Orcidhttp://orcid.org/0000-0003-1876-7712
  • , 
  • Victor Fung
    Victor Fung
    Department of Chemistry, University of California, Riverside, California 92521, United States
    More by Victor Fung
  • , 
  • Xun Yuan*
    Xun Yuan
    College of Materials Science and Engineering, Qingdao University of Science and Technology, Qingdao 266042, P. R. China
    *[email protected]
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  • , 
  • De-en Jiang
    De-en Jiang
    Department of Chemistry, University of California, Riverside, California 92521, United States
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    Orcidhttp://orcid.org/0000-0001-5167-0731
  • , and 
  • Jianping Xie*
    Jianping Xie
    Department of Chemical and Biomolecular Engineering, National University of Singapore, 4 Engineering Drive 4, 117585 Singapore
    Joint School of National University of Singapore and Tianjin University, International Campus of Tianjin University, Binhai New City, Fuzhou 350207, P. R. China
    *[email protected]
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    Orcidhttp://orcid.org/0000-0002-3254-5799
Cite this: J. Am. Chem. Soc. 2019, 141, 48, 18977–18983
Publication Date (Web):October 14, 2019
https://doi.org/10.1021/jacs.9b05776
Copyright © 2019 American Chemical Society
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    Abstract

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    Alloying metal materials with heterometal atoms is an efficient way to diversify the function of materials, but in-depth understanding of the dynamic heterometallic diffusion inside the alloying materials is rather limited, especially at the atomic level. Here, we report the real-time monitoring of the dynamic diffusion process of a single gold (Au) atom into an atomically precise silver nanocluster (Ag NC), Ag25(MHA)18 (MHA = 6-mercaptohexanoic acid), by using in situ UV–vis absorption spectroscopy in combination with mass and tandem mass spectrometry. We found that the Au heteroatom first replaces the Ag atom at the surface Ag2(MHA)3 motifs of Ag25(MHA)18. After that, the Au atom diffuses into the surface layer of the icosahedral Ag13 kernel and finally occupies the center of the alloy NCs to form the thermodynamically stable Au@Ag24(MHA)18 product. Density functional theory (DFT) calculations reveal that the key thermodynamic driving force is the preference of the Au heteroatom for the central site of alloy NCs. The real-time monitoring approach developed in this study could also be extended to other metal alloy systems to reveal the reaction dynamics of intracluster diffusion of heteroatoms, as well as the formation mechanisms of metal alloy nanomaterials.

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/jacs.9b05776.

    • Figures of ESI mass spectra, UV–vis absorption, isotope analysis of the fragments, tandem mass spectra, XPS spectra, and energy profiles and transition state structures (PDF)

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