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

Qiaofeng Yao, Victor Fung, Cheng Sun, Sida Huang, Tiankai Chen, Jiang De-en, Jim Yang Lee and Jianping Xie ()
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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
Jiang De-en: University of California
Jim Yang Lee: National University of Singapore
Jianping Xie: National University of Singapore

Nature Communications, 2018, vol. 9, issue 1, 1-11

Abstract: 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.

Date: 2018
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DOI: 10.1038/s41467-018-04410-6

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