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Revealing isoelectronic size conversion dynamics of metal nanoclusters by a noncrystallization approach

Author

Listed:
  • Qiaofeng Yao

    (National University of Singapore)

  • Victor Fung

    (University of California)

  • Cheng Sun

    (National University of Singapore)

  • Sida Huang

    (National University of Singapore)

  • Tiankai Chen

    (National University of Singapore)

  • De-en Jiang

    (University of California)

  • Jim Yang Lee

    (National University of Singapore)

  • Jianping Xie

    (National University of Singapore)

Abstract

Atom-by-atom engineering of nanomaterials requires atomic-level knowledge of the size evolution mechanism of nanoparticles, which remains one of the greatest mysteries in nanochemistry. Here we reveal atomic-level dynamics of size evolution reaction of molecular-like nanoparticles, i.e., nanoclusters (NCs) by delicate mass spectrometry (MS) analyses. The model size-conversion reaction is [Au23(SR)16]− → [Au25(SR)18]− (SR = thiolate ligand). We demonstrate that such isoelectronic (valence electron count is 8 in both NCs) size-conversion occurs by a surface-motif-exchange-induced symmetry-breaking core structure transformation mechanism, surfacing as a definitive reaction of [Au23(SR)16]− + 2 [Au2(SR)3]− → [Au25(SR)18]− + 2 [Au(SR)2]−. The detailed tandem MS analyses further suggest the bond susceptibility hierarchies in feed and final Au NCs, shedding mechanistic light on cluster reaction dynamics at atomic level. The MS-based mechanistic approach developed in this study also opens a complementary avenue to X-ray crystallography to reveal size evolution kinetics and dynamics.

Suggested Citation

  • Qiaofeng Yao & Victor Fung & Cheng Sun & Sida Huang & Tiankai Chen & De-en Jiang & Jim Yang Lee & Jianping Xie, 2018. "Revealing isoelectronic size conversion dynamics of metal nanoclusters by a noncrystallization approach," Nature Communications, Nature, vol. 9(1), pages 1-11, December.
  • Handle: RePEc:nat:natcom:v:9:y:2018:i:1:d:10.1038_s41467-018-04410-6
    DOI: 10.1038/s41467-018-04410-6
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